HIGH-SILICA Y MOLECULAR SIEVE HAVING FAU TOPOLOGY AND PREPARATION METHOD THEREFOR

Abstract

Disclosed in the present application is a high-silica Y molecular sieve having FAU topology. The anhydrous chemical constitution of the molecular sieve is as shown in formula I: kM.mR1.nR2.(Si.sub.xAl.sub.y)O.sub.2 Formula I; wherein, M is at least one of alkali metal elements; R1 and R2 represent organic templating agent agents; k represents the numbers of moles of the alkali metal element corresponding to per mole of (Si.sub.xAl.sub.y)O.sub.2, k=0˜0.20; m and n represent the numbers of moles of templating agents R1 and R2 corresponding to per mole of (Si.sub.xAl.sub.y)O.sub.2, m=0˜0.20, n=0.01˜0.20; x, y respectively represents the mole fraction of Si and Al, 2x/y=7-40, and x+y=1; R1, R2 are independently selected from one of nitrogen-containing heterocyclic compounds and their derivatives, and quaternary ammonium compounds. Also disclosed in the present application is a synthesis method for the high-silica Y molecular sieve having FAU topology.

Claims

1-45. (canceled)

46. A high-silica Y molecular sieve having FAU topology, wherein the anhydrous chemical constitution of the molecular sieve is as shown in formula I:
kM.mR1.nR2.(Si.sub.xAl.sub.y)O.sub.2  Formula I wherein, M is at least one of alkali metal elements; R1 and R2 represent organic templating agents; k represents the number of moles of alkali metal element M per mole (Si.sub.xAl.sub.y)O.sub.2, k=0˜0.20; m and n represent the number of moles of templating agents R.sup.1 and R.sup.2 per mole of (Si.sub.xAl.sub.y)O.sub.2, m=0˜0.20, n=0.01˜0.20; x and y respectively represent the mole fractions of Si and Al, 2x/y=7˜40, and x+y=1; R.sup.1 and R.sup.2 are independently one of nitrogen-containing heterocyclic compounds and derivatives thereof, and quaternary ammonium compounds; a structural formula of the quaternary ammonium compound is as shown in formula II; ##STR00006## in formula II, R.sup.21, R.sup.22, R.sup.23 and R.sup.24 are independently at least one of C.sub.1˜C.sub.12 alkyl, C.sub.1˜C.sub.12 alkoxy, C.sub.1˜C.sub.12 hydroxyalkyl, aryl and adamantyl; X.sup.n− is one of OH.sup.−, Cl.sup.−, Br.sup.−, I.sup.−, NO.sub.3.sup.−, HSO.sub.4.sup.−, H.sub.2PO.sub.3.sup.−, SO.sub.4.sup.2−, HPO.sub.3.sup.2−, and PO.sub.3.sup.3−.

47. The high-silica Y molecular sieve having FAU topology according to claim 46, wherein M is at least one of Na, K, and Cs, and 2x/y=7˜30; preferably, M is at least one of Na, K, and Cs, and 2x/y=8˜30; preferably, k=0.01˜0.15; m=0.01˜0.1; n=0.02˜0.15; more preferably, k=0.02˜0.13; m=0.01˜0.04; n=0.03˜0.08.

48. The high-silica Y molecular sieve having FAU topology according to claim 46, wherein R.sup.1 and R.sup.2 are independently at least one of quaternary ammonium compounds; preferably, R.sup.1 and R.sup.2 are independently at least one of tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, tetrapentylammonium hydroxide, tetrahexylammonium hydroxide, tetrapropylammonium bromide, tetrabutylammonium chloride, tetrapentylammonium bromide, tripropyl-isobutylammonium bromide, tributyl-cyclohexylammonium hydroxide, dibutyl-dihexyl ammonium hydroxide, choline, triethyl-hydroxyethyl ammonium hydroxide, tripropyl-hydroxyethyl ammonium hydroxide, tributyl-hydroxyethyl ammonium hydroxide, tributyl-benzyl ammonium hydroxide, triethyl-benzyl ammonium hydroxide, tripropyl-benzyl ammonium hydroxide, N,N,N-triethyl-adamantyl ammonium chloride, and N,N,N-tripropyl-adamantyl ammonium chloride; preferably, R.sup.1 is at least one of tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide and choline, R.sup.2 is at least one of tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, tetrapentylammonium hydroxide, tetrahexylammonium hydroxide, tetrapropylammonium bromide, tetrabutylammonium chloride, tetrapentylammonium bromide, tripropyl-isobutyl ammonium bromide, tributyl-cyclohexylammonium hydroxide, dibutyl-dihexyl ammonium hydroxide, choline, triethyl-hydroxyethyl ammonium hydroxide, tripropyl-hydroxyethyl ammonium hydroxide, tributyl-hydroxyethyl ammonium hydroxide, tributyl-benzyl ammonium hydroxide, triethyl-benzyl ammonium hydroxide, tripropyl-benzyl ammonium hydroxide, N,N,N-triethyl-adamantyl ammonium chloride, and N,N,N-tripropyl-adamantyl ammonium chloride.

49. The high-silica Y molecular sieve having FAU topology according to claim 46, wherein R.sup.1 is at least one of quaternary ammonium compounds; R.sup.2 is at least one of nitrogen-containing heterocyclic compounds and derivatives thereof; preferably, R.sup.1 is at least one of tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide and choline, and R.sup.2 is at least one of nitrogen-containing heterocyclic compounds and derivatives thereof; preferably, R.sup.2 is at least one of pyridine, N-methylpyridine, N-ethylpyridine, N-propylpyridine, N-butylpyridine, N-ethyl-3-butylpyridine, 1-ethyl-2-propylpyridine hydroxide, piperidine, N,N-dimethylpiperidine, N,N-dimethyl-3,5-diethylpiperidine hydroxide, N,N-dimethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-2,6-dimethylpiperidine hydroxide, N,N-dimethyl-2,6-diethylpiperidine hydroxide, imidazole, 1-ethyl-3-butylimidazole hydroxide, 1-ethyl-3-butyl-4-propylimidazole hydroxide, 1-benzyl-3-methylimidazole hydroxide, 1-benzyl-3-ethylimidazole hydroxide, 1-benzyl-3-butylimidazole hydroxide, piperazine, N-methylpiperazine, 1,4-dipropylpiperazine, 1-methyl-4-ethylpiperazine, and 1-ethyl-4-butyl-5-methylpiperazine.

50. A method for preparing high-silica Y molecular sieve having FAU topology comprising following steps: a) mixing raw materials containing aluminum source, silicon source, alkali metal source, organic templating agent R and water to prepare an initial gel mixture I, wherein the aluminum source, silicon source, alkali metal source, organic templating agent R and water in the raw materials have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=10˜200; M.sub.2O/Al.sub.2O.sub.3=0˜30, wherein M is at least one of alkali metal elements; R/Al.sub.2O.sub.3=1˜45; H.sub.2O/Al.sub.2O.sub.3=50˜8000; b) adding silica-alumina molecular sieve seed crystal having FAU or EMT topology to the initial gel mixture I obtained in step a) to obtain a mixture II; c) placing the mixture II obtained in step b) in a sealed reactor to perform crystallization to obtain the high-silica Y molecular sieve having FAU topology; wherein, the number of moles of silicon source is calculated by SiO.sub.2; the number of moles of aluminum source is calculated by Al.sub.2O.sub.3; the number of moles of templating agent R is calculated by the number of moles of R itself; and the number of moles of alkali metal source is calculated by the number of moles of corresponding metal oxide M.sub.2O.

51. The method according to claim 50, wherein, in step a), H.sub.2O/Al.sub.2O.sub.3=50˜6000; preferably, in step a), H.sub.2O/Al.sub.2O.sub.3=100˜8000; preferably, in step a), R/Al.sub.2O.sub.3=0.1˜25.

52. The method according to claim 50, wherein, in step a), the organic templating agent R is at least one of nitrogen-containing heterocyclic compounds and derivatives thereof, and quaternary ammonium compounds; the structural formula of the quaternary ammonium compound is as shown in formula II; ##STR00007## in formula II, R.sup.21, R.sup.22, R.sup.23 and R.sup.24 are independently at least one of C.sub.1˜C.sub.12 alkyl, C.sub.1˜C.sub.12 alkoxy, C.sub.1˜C.sub.12 hydroxyalkyl, aryl and adamantyl; X.sup.n− is one of OH.sup.−, Cl.sup.−, Br.sup.−, I.sup.−, NO.sub.3.sup.−, HSO.sub.4.sup.−, H.sub.2PO.sub.3.sup.−, SO.sub.4.sup.2−, HPO.sub.3.sup.2−, and PO.sub.3.sup.3−; preferably, the organic templating agent R in step a) is at least one of tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, tetrapentylammonium hydroxide, tetrahexylammonium hydroxide, tetrapropylammonium bromide, tetrabutylammonium chloride, tetrapentylammonium bromide, tripropyl-isobutyl ammonium bromide, tributyl-cyclohexylammonium hydroxide, dibutyl-dihexyl ammonium hydroxide, choline, triethyl-hydroxyethyl ammonium hydroxide, tripropyl-hydroxyethyl ammonium hydroxide, tributyl-hydroxyethyl ammonium hydroxide, tributyl-benzyl ammonium hydroxide, triethyl-benzyl ammonium hydroxide, tripropyl-benzyl ammonium hydroxide, N,N,N-triethyl-adamantyl ammonium chloride, and N,N,N-tripropyl-adamantyl ammonium chloride; preferably, the nitrogen-containing heterocyclic templating agent R in step a) is at least one of nitrogen-containing heterocyclic compounds and derivatives thereof; preferably, the nitrogen-containing heterocyclic templating agent R in step a) is at least one of pyridine, N-methylpyridine, N-ethylpyridine, N-propylpyridine, N-butylpyridine, N-ethyl-3-butylpyridine, 1-ethyl-2-propylpyridine hydroxide, piperidine, N,N-dimethylpiperidine, N,N-dimethyl-3,5-diethylpiperidine hydroxide, N,N-dimethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-2,6-dimethylpiperidine hydroxide, N,N-dimethyl-2,6-diethylpiperidine hydroxide, imidazole, 1-ethyl-3-butylimidazole hydroxide, 1-ethyl-3-butyl-4-propylimidazole hydroxide, 1-benzyl-3-methylimidazole hydroxide, 1-benzyl-3-ethylimidazole hydroxide, 1-benzyl-3-butylimidazole hydroxide, piperazine, N-methylpiperazine, 1,4-dipropylpiperazine, 1-methyl-4-ethylpiperazine, and 1-ethyl-4-butyl-5-methylpiperazine.

53. The method according to claim 50, wherein the silicon source in step a) is at least one of methyl ortho silicate, ethyl orthosilicate, silica sol, solid silica gel, fumed silica, and sodium silicate; the aluminum source in step a) is at least one of sodium aluminate, aluminum oxide, aluminum hydroxide, aluminum isopropoxide, aluminum 2-butoxide, aluminum chloride, aluminum sulfate, aluminum nitrate, and pseudo-boehmite; the alkali metal source in step a) is at least one of sodium hydroxide, potassium hydroxide, and cesium hydroxide.

54. The method according to claim 50, wherein step a) comprises mixing the aluminum source, the alkali metal source, the organic templating agent R and water, and then adding the silicon source to mix to obtain the initial gel mixture I.

55. The method according to claim 50, wherein the aluminum source, silicon source, alkali metal source, organic templating agent R and water in the raw materials in step a) have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=10˜200; M.sub.2O/Al.sub.2O.sub.3=0˜30, wherein M is at least one of alkali metal elements; R/Al.sub.2O.sub.3=1˜45; H.sub.2O/Al.sub.2O.sub.3=100˜6000.

56. The method according to claim 50, wherein a weight ratio of silica alumina molecular sieve seed crystal having FAU or EMT topology added in the mixture II in step b), to the silicon source in the initial gel mixture I ranges from 0.01:1 to 0.3:1; wherein, the weight of the silicon source in the initial gel mixture I is calculated by the weight of SiO.sub.2; preferably, a silica-alumina molar ratio SiO.sub.2/Al.sub.2O.sub.3 of the silica-alumina molecular sieve seed crystal having FAU or EMT topology in step b) is 2˜∞; preferably, a silica-alumina molar ratio SiO.sub.2/Al.sub.2O.sub.3 of the silica-alumina molecular sieve seed crystal having FAU or EMT topology in step b) ranges from 2.5 to 200.

57. The method according to claim 50, wherein a crystallization temperature in step c) ranges from 90 to 180° C., and a crystallization time in step c) ranges from 0.1 to 15 days; preferably, the crystallization in step c) is performed dynamically or statically.

58. A method for preparing high-silica Y molecular sieve having FAU topology, comprising following steps: a) mixing raw materials I containing aluminum source A.sup.1, silicon source Si.sup.1, alkali metal source M.sup.1, organic templating agent R.sup.1 and water, and aging to obtain a directing agent; wherein, the aluminum source A.sup.1, silicon source Si.sup.1, alkali metal source M.sup.1, organic templating agent R.sup.1 and water in the raw materials I have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=5˜30; M.sup.1.sub.2O/Al.sub.2O.sub.3=0˜7, wherein M.sup.1 is at least one of alkali metal elements; R.sup.1/Al.sub.2O.sub.3=1˜40; H.sub.2O/Al.sub.2O.sub.3=100˜600; b) mixing raw materials II containing aluminum source A.sup.2, silicon source Si.sup.2, alkali metal source M.sup.2, organic templating agent R.sup.2, and water to prepare an initial gel; wherein, the aluminum source A.sup.2, silicon source Si.sup.2, alkali metal source M.sup.2, organic templating agent R.sup.2 and water in the raw materials II have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=10˜200; M.sup.2.sub.2O/Al.sub.2O.sub.3=0˜30, wherein M.sup.2 is at least one of alkali metal elements; R.sup.2/Al.sub.2O.sub.3=1˜45; H.sub.2O/Al.sub.2O.sub.3=100˜8000; c) adding the directing agent in step a) to the initial gel in step b) and, after mixing uniformly, placing the obtained mixture in a sealed reactor for crystallization to obtain the high-silica Y molecular sieve having FAU topology; wherein, the number of moles of silicon source Si.sup.1 and Si.sup.2 is respectively calculated by SiO.sub.2; the number of moles of aluminum source A.sup.1 and A.sup.2 is respectively calculated by Al.sub.2O.sub.3; the number of moles of templating agent R.sup.1 and R.sup.2 is respectively calculated by the number of moles of themselves; and the number of moles of alkali metal source M.sup.1 and M.sup.2 is respectively calculated by the number of moles of corresponding metal oxide M.sup.1.sub.2 and M.sup.2.sub.2O.

59. The method according to claim 58, wherein the aluminum source A.sup.1, silicon source Si.sup.1, alkali metal source M.sup.1, organic templating agent R.sup.1 and water in the raw materials I in step a) have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=5˜30; M.sup.1.sub.2O/Al.sub.2O.sub.3=0˜3, wherein M.sup.1 is at least one of alkali metal elements; R.sup.1/Al.sub.2O.sub.3=5˜40; H.sub.2O/Al.sub.2O.sub.3=100˜600; preferably, the aluminum source A.sup.2, silicon source Si.sup.2, alkali metal source M.sup.2, organic templating agent R.sup.2, and water in the raw material II in step b) have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=10˜200; M.sup.2.sub.2O/Al.sub.2O.sub.3=0˜30, wherein M.sup.2 is at least one of alkali metal elements; R.sup.2/Al.sub.2O.sub.3=1˜45; H.sub.2O/Al.sub.2O.sub.3=100˜4000; preferably, the silicon sources Si.sup.1 and Si.sup.2 in step a) and step b) are independently at least one of methyl orthosilicate, ethyl orthosilicate, silica sol, solid silica gel, fumed silica, and sodium silicate; the aluminum sources A.sup.1 and A.sup.2 in step a) and step b) are independently at least one of sodium aluminate, aluminum oxide, aluminum hydroxide, aluminum isopropoxide, aluminum 2-butoxide, aluminum chloride, aluminum sulfate, aluminum nitrate and pseudo-boehmite; the alkali metal sources M.sup.1 and M.sup.2 in step a) and step b) are independently at least one of sodium hydroxide, potassium hydroxide, and cesium hydroxide.

60. The method according to claim 58, wherein the organic templating agents R.sup.1 and R.sup.2 in step a) and step b) are independently one of nitrogen-containing heterocyclic compounds and derivatives thereof, and quaternary ammonium compounds; the structural formula of the quaternary ammonium compound is as shown in formula II; ##STR00008## in formula II, R.sup.21, R.sup.22, R.sup.23 and R.sup.24 are independently at least one of C.sub.1˜C.sub.12 alkyl, C.sub.1˜C.sub.12 alkoxy, C.sub.1˜C.sub.12 hydroxyalkyl, aryl and adamantyl; X.sup.n− is one of OH.sup.−, Cl.sup.−, Br.sup.−, I.sup.−, NO.sub.3.sup.−, HSO.sub.4.sup.−, H.sub.2PO.sub.3.sup.−, SO.sub.4.sup.2−, HPO.sub.3.sup.2−, and PO.sub.3.sup.3−; preferably, R.sup.1 and R.sup.2 are independently at least one of tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, tetrapentylammonium hydroxide, tetrahexylammonium hydroxide, tetrapropylammonium bromide, tetrabutylammonium chloride, tetrapentylammonium bromide, tripropyl-isobutylammonium bromide, tributyl-cyclohexylammonium hydroxide, dibutyl-dihexylammonium hydroxide, choline, triethyl-hydroxyethyl ammonium hydroxide, tripropyl-hydroxyethyl ammonium hydroxide, tributyl-hydroxyethyl ammonium hydroxide, tributyl-benzyl ammonium hydroxide, triethyl-benzyl ammonium hydroxide, tripropyl-benzyl ammonium hydroxide, N,N,N-triethyl-adamantyl ammonium chloride, and N,N,N-tripropyl-adamantyl ammonium chloride; preferably, R.sup.1 is at least one of tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide, and choline; R.sup.2 is at least one of tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, tetrapentylammonium hydroxide, tetrahexylammonium hydroxide, tetrapropylammonium bromide, tetrabutylammonium chloride, tetrapentylammonium bromide, tripropyl-isobutylammonium bromide, tributyl-cyclohexylammonium hydroxide, dibutyl-dihexyl ammonium hydroxide, choline, triethyl-hydroxyethyl ammonium hydroxide, tripropyl-hydroxyethyl ammonium hydroxide, tributyl-hydroxyethyl ammonium hydroxide, tributyl-benzyl ammonium hydroxide, triethyl-benzyl ammonium hydroxide, tripropyl-benzyl ammonium hydroxide, N,N,N-triethyl-adamantyl ammonium chloride, and N,N,N-tripropyl-adamantyl ammonium chloride; Preferably, wherein R.sup.2 is at least one of pyridine, N-methylpyridine, N-ethylpyridine, N-propylpyridine, N-butylpyridine, N-ethyl-3-butylpyridine, 1-ethyl-2-propylpyridine hydroxide, piperidine, N,N-dimethylpiperidine, N,N-dimethyl-3,5-diethylpiperidine hydroxide, N,N-dimethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-3,5-dipropylpiperidine hydroxide, N,N-diethyl-2,6-dimethylpiperidine hydroxide, N,N-dimethyl-2,6-diethylpiperidine hydroxide, imidazole, 1-ethyl-3-butylimidazole hydroxide, 1-ethyl-3-butyl-4-propylimidazole hydroxide, 1-benzyl-3-methylimidazole hydroxide, 1-benzyl-3-ethylimidazole hydroxide, 1-benzyl-3-butylimidazole hydroxide, piperazine, N-methylpiperazine, 1,4-dipropylpiperazine, 1-methyl-4-ethylpiperazine, and 1-ethyl-4-butyl-5-methylpiperazine.

61. The method according to claim 58, wherein an aging temperature in step a) ranges from 25 to 140° C. for an aging time in a range from 0.5 to 30 days; preferably, an aging temperature in step a) ranges from 25 to 140° C. for an aging time in a range from 1 to 30 days; preferably, an aging temperature in step a) ranges from 30 to 120° C. for an aging time in a range from 1 to 25 days.

62. The method according to claim 58, wherein the aging in step a) is a two-stage aging, a temperature for a first stage aging ranges from 30 to 40° C., a time for the first stage aging ranges from 0.5 to 5 days while a temperature for the second stage aging ranges from 50 to 100° C., and a time for second-stage aging ranges from 2 to 8 days.

63. The method according to claim 58, wherein step a) comprises: mixing the aluminum source A.sup.1, the alkali metal source M.sup.1, the organic templating agent R.sup.1 and water uniformly, adding the silicon source S.sup.1 therein, stirring, mixing and then aging, wherein an aging temperature ranges from 25 to 140° C., and an aging time ranges from 1 to 30 days to obtain the directing agent.

64. The method according to claim 58, wherein the aluminum source A.sup.2, the silicon source Si.sup.2, the alkali metal source M.sup.2, the organic templating agent R.sup.2, and water in step b) have the following molar ratios: SiO.sub.2/Al.sub.2O.sub.3=10˜200; M.sup.2.sub.2O/Al.sub.2O.sub.3=0˜30, wherein M.sup.2 is at least one of alkali metal elements; R.sup.2/Al.sub.2O.sub.3=1˜45; H.sub.2O/Al.sub.2O.sub.3=100˜6000.

65. The method according to claim 58, wherein, a weight ratio of silica in the directing agent to silica in the initial gel in step c) ranges from 0.01:1 to 0.3:1; preferably, a weight ratio of silica in the directing agent to silica in the initial gel in step c) ranges from 0.01:1 to 0.2:1; preferably, a crystallization temperature in step c) ranges from 90 to 180° C. for a crystallization time in a range from 1 to 15 days; a crystallization temperature in step c) ranges from 90 to 140° C. for a crystallization time in a range from 3 to 15 days; preferably, the crystallization in step c) is performed dynamically and/or statically.

Description

BRIEF DESCRIPTION OF DRAWINGS

[0244] FIG. 1 is X-ray diffraction (XRD) spectrum of sample X #1.

[0245] FIG. 2 is scanning electron not microscope (SEM) image of sample X #1.

[0246] FIG. 3 is silicon nuclear magnetic (.sup.29Si-NMR) spectrum of sample X #1.

[0247] FIG. 4 is X-ray diffraction (XRD) spectrum of sample V #1.

[0248] FIG. 5 is X-ray diffraction (XRD) spectrum of sample X1.

[0249] FIG. 6 is scanning electron microscole (SEM) image of sample X1.

[0250] FIG. 7 is silicon nuclear magnetic (.sup.29Si-NMR) spectrum of sample X1.

[0251] FIG. 8 is X-ray diffraction (XRD) spectrum of the comparative sample V1.

[0252] FIG. 9 is X-ray diffraction (XRD) spectrum of sample Y #1.

[0253] FIG. 10 is scanning electron microscope (SEM) image of sample Y #1.

[0254] FIG. 11 is silicon nuclear magnetic (.sup.29Si-NMR) spectrum of sample Y #1.

[0255] FIG. 12 is X-ray diffraction (XRD) spectrum of sample S1.

[0256] FIG. 13 is X-ray diffraction (XRD) spectrum of simple T1.

[0257] FIG. 14 is an X-ray diffraction (XRD) spectrum of sample Y1.

[0258] FIG. 15 is scanning electron scope (SEM) image of sample Y1.

[0259] FIG. 16 is silicon electron microscope (.sup.29Si-NMR) spectrum of sample Y1.

[0260] FIG. 17 is X-ray diffraction (XRD) spectrum of the comparative sample S1.

[0261] FIG. 18 is X-ray diffraction (XRD) spectrum of the comparative sample T1.

DETAILED DESCRIPTION

[0262] The present application will be described in detail below with reference to the examples, but the present application is not limited to these examples.

[0263] The analysis methods in the examples of the present application are as follows.

[0264] The X-ray powder diffraction phase analysis (XRD) of the product adopts to XPert PRO X-ray diffraction from PANalytical, the Netherlands. Cu target, Kα radiation source (λ=0.15418 nm), voltage 40 KV, current mA.

[0265] The instrument used in the scanning electron microscope (SEM) test is Hirachi SU8020 emission scanning electron microscope, and the accelerating voltage is 2 kV.

[0266] The elemental constitution was measured by Philips Magix 2424 X-ray fluorescence analyzer (XRF).

[0267] The silicon nuclear magnet (.sup.29Si-NMR) experiment was carried out on a Braker Avance III 600 (14.1 Tesla) spectrometer using a 7 mm double resonance probe with a rotation speed of 6 kHz. Using high-power proton decoupling program, sampling times are 1024, ×4 pulse width is 2.5 μs, sampling delay is 10 s, and 4,4-dimethyl-4-propanesulfonate (DSS) is used as chemical shift reference which is calibrated to be 0 ppm.

[0268] The carbon nuclear magnetic (.sup.13C MAS NMR) experiment was carried out on a Braker Avance III 600 (14.1 Tesla) spectrometer using a 4 mm triple resonance probe with a rotation speed of 12 kHz, wherein amantadine was used as the chemical shift reference which was calibrated to be 0 ppm.

Example 1: Preparation of Sample X #1

[0269] Preparation of synthetic gel: 0.7 g sodium aluminate (Al.sub.2O.sub.3:48.3 wt %, Na.sub.2O: 35.3 wt %, China National Pharmaceutical (Group) Shanghai chemical Reagent Company), 0.20 g sodium hydroxide, 13.0 g tetrapropylammonium (25 wt %) were dissolved in 2.40 g deionized water and stirred until to be clear. 13.3 g silica gel (SiO.sub.2: 30 wt %, Shenyang Chemical Co., Ltd) was added therein dropwise and stirred for 0.5 hour. Then 0.4 g Y zeolite as seed crystal with silica-alumina ratio of 3 was added, and stirring was continued for 2 hours.

[0270] Synthesis of high-silica Y zeolite: The synthetic gel was transferred into a stainless-steel reactor, and was subject to rotational crystallization at 130° C. for 5 days. After the crystallization was completed, the obtained solid was separated from liquid, washed to be neutrality, then dried at 100° C. for 12 hours. The obtained sample was denoted as sample X #1.

[0271] X-ray diffraction (XRD) spectrum of sample X #1 is shown in FIG. 1, demonstrating that the sample X #1 is molecular sieve having FAU framework structure. Scanning electron microscope (SEM) image thereof is shown in FIG. 2, demonstrating that the particles of sample X #1 are small pieces with a size rangy from 50 nm to 200 nm. .sup.29Si MAS NMR spectrum thereof is shown in FIG. 3. The firting calculation shows that the silica-alumina ratio in the framework is consistent with the calculation results conducted by XRF. According to the XRF and .sup.13C MAS NMR normalization analysis, the element of constitution of sample X #1 is 0.07Na.0.07R2.sup.1.(Si.sub.0.86Al.sub.0.14)O.sub.2, where R2.sup.1 is tetrapropylammonium hydroxide.

Example 2 Preparation of Samples X #2-X #30

[0272] The preparation process of any one of samples X #2-X #30 is the same as that of Example 1. The raw materials for preparing samples X #2-X #30, molar ratio thereof, addition amount of seed crystal (weight ratio of seed crystal to SiO.sub.2 in gel), crystallization conditions, crystal structure, silica-alumina ration (the silica-alumina ratio of the obtained product is measured by X-ray fluorescence analyzer (XRF)) and the product constitutent are shown in Table 1.

[0273] Samples X #1-X #20 were prepared using silica-alumina molecular sieves having FAU topology as seed crystals, of which silica-alumina ratios were 3, 2.8. 3. 3.5, 45. 6. 6, 6, 6, 7, 70, 10. 4. 5, 6, 8, 3.5, 35, 12. 20 respectively, and which were purchased from Zibo Rumxin Chemical Technology Co., Ltd. Samples X #21-X #30 were prepared using silica-alumina molecular sieves having EMT topology as seed crystals, of which silica-alumina ratios were 10, 8, 8.5, 7, 7, 8, 21, 7, 8, 22 respectively, and which were purchased from Henan Huanyu Molecular Sieve Co., Ltd.

Comparative Example 1 Preparation of Comparative Samples V #1-V #30

[0274] The specific types of raw materials for preparing synthetic gel, molar ratio thereof, preparation process and crystallization conditions are the same as those of sample X #1 in Example 1, except than the seed crystal addition step is omitted. The specific types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of the product are shown in Table 2. The obtained samples are denoted as comparative samples V #1-V #30.

Example 3 Characterization and Analysis of Sample X #1-X #30 and Comparative Samples V #1-V #30

[0275] The phases of samples X #1-X #30 and comparative samples V #1-V #30 were analyzed by X-ray diffraction method.

[0276] The results show that each of the samples X #1-X #30 prepared in Examples 1 and 2 is Y molecular sieve with both high purity and high crystallinity. The XRD spectrum of sample X #1 as typical representative is shorn in FIG. 1, SEM image thereof is shown in FIG. 2, and Si NMR thereof is shown in FIG. 3. The XRD spectrum result of any one of samples X #2-X30 is close to FIG. 1. In other words, the diffraction peak positions and shapes are substantially identical. The relative peak intensity fluctuates within ±5% depending on the change of synthesis conditions, demonstrating that any of samples X #1-X #30 has the structural characteristics of Y zeolite and has no impurities. The silica-alumina ratio of any sample is much higher than that of conventional Y zeolite. The introduction of organic templating agent is the key to the synthesis of high-silica Y zeolite.

[0277] Each of V #1-V #30 as products in Table 2 is amorphous, and the XRD spectrum of the comparative sample V #1 as typical represenative is shown in FIG. 4. It can be seen that during the synthesis of high-silica Y zeolite, in addition to the organic templating agent, the introduction of seed crystal is also necessary.

TABLE-US-00001 TABLE 1 Types of raw materials, molar ratio thereof, addition amount of seed crystal, crystallization conditions, crystal structure, silica-alumina ratio and product constitution of samples X#1-X#30 Addition amount Crystal- Crystal- Silica- of seed lization lization Crystal alumina Sample Initial gel constitution crystal temperature time structure ratio Product constitution X#1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:4.8R2.sup.1:360H.sub.2O  1% 130° C. Dynamic FAU 12 0.07Na0.07R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3.6R2.sup.1:200H.sub.2O  3% 130° C. Static FAU 9 0.09Na0.09R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 4 days X#3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5.2R2.sup.1:400H.sub.2O 12% 110° C. Dynamic FAU 11 0.07Na0.08R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X#4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13R2.sup.2:800H.sub.2O  8% 140° C. Dynamic FAU 15 0.03Na0.07R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X#5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.2:400H.sub.2O 15% 120° C. Static FAU 8 0.08Na0.12R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X#6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5R2.sup.3:400H.sub.2O 10% 130° C. Static FAU 11 0.07Na0.08R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X#7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :25Na.sub.2O:45R2text missing or illegible when filed :3000H.sub.2O 12% 120° C. Dynamic FAU 28 0.02Na0.05R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X#8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:11R2text missing or illegible when filed :800H.sub.2O  8% 140° C. Dynamic FAU 18 0.03Na0.07R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X#9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:15R2text missing or illegible when filed :900H.sub.2O  9% 140° C. Dynamic FAU 20 0.03Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 2 days X#10 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :20Cs.sub.2O:10R2.sup.4:800H.sub.2O  5% 180 Dynamic FAU 35 0.01Cs0.02R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 0.2 day X#11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R2.sup.4:500H.sub.2O 14% 120° C. Static FAU 13 0.07Na0.06R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X#12 150SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :15K.sub.2O:20R2.sup.4:1500H.sub.2O 16% 160° C. Dynamic FAU 40 0.01K0.01R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 0.5 day X#13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R2text missing or illegible when filed :500H.sub.2O 20% 100° C. Static FAU 13 0.09Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X#14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25R2text missing or illegible when filed :2000H.sub.2O 16% 120° C. Dynamic FAU 20 0.04Na0.05R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#15 150SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:35R2text missing or illegible when filed :2800H.sub.2O 17% 120° C. Dynamic FAU 25 0.03Na0.04R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#16 80SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2text missing or illegible when filed :1500H.sub.2O 10% 110° C. Dynamic FAU 18 0.04Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#17 100SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:23R2text missing or illegible when filed :1800H.sub.2O  9% 115° C. Dynamic FAU 20 0.03Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#18 60SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15R2text missing or illegible when filed :1100H.sub.2O  7% 130° C. Dynamic FAU 15 0.06Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X#19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9R2text missing or illegible when filed :800H.sub.2O 13% 120° C. Static FAU 14 0.06Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X#20 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:5R2text missing or illegible when filed :150H.sub.2O 16% 90° C. Static FAU 7 0.13Na0.09R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 15 days X#21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5R2text missing or illegible when filed :200H.sub.2O 10% 140° C. Static FAU 8 0.11Na0.09R2.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8R2text missing or illegible when filed :400H.sub.2O 12% 110° C. Static FAU 12 0.09Na0.05R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2text missing or illegible when filed :800H.sub.2O 12% 120° C. Dynamic FAU 20 0.03Na0.06R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X#24 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 15% 140° C. Dynamic FAU 12 0.08Na0.06R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2text missing or illegible when filed :280H.sub.2O 10% 110° C. Dynamic FAU 10 0.09Na0.08R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 4 days X#26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2.sup.10:2000H.sub.2O 12% 120° C. Dynamic FAU 20 0.04Na0.05R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:30R2.sup.10:2800H.sub.2O 11% 120° C. Dynamic FAU 30 0.02Na0.04R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X#28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.11:1500H.sub.2O 10% 120° C. Dynamic FAU 16 0.04Na0.07R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 4 days X#29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2.sup.11:1500H.sub.2O  9% 120° C. Dynamic FAU 12 0.06Na0.08R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X#30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :14Na.sub.2O:25R2.sup.11:2500H.sub.2O 10% 120° C. Dynamic FAU 25 0.02Na0.05R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum 2-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R2.sup.1: Tetrapropylammonium hydroxide R2.sup.2: Triethylhexylammonium hydroxide R2.sup.3: Triethylbenzylammonium hydroxide R2.sup.4: N,N,N-tripropyl adamantylammonium hydroxide R2.sup.5: Dipropyldibutylammonium hydroxide R2.sup.6: Benzyltriporpylammonium hydroxide R2.sup.7: Choline R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Tributyl-hydroxyethyl ammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00002 TABLE 2 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples V#1-V#30 Crystallization Crystallization Crystal Sample Initial gel constitution temperature manner and time structure V#1 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:4.8R2text missing or illegible when filed :360H.sub.2O 130° C. Dynamic 5 days Amorphous V#2 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3.6R2text missing or illegible when filed :200H.sub.2O 130° C. Static 4 days Amorphous V#3 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5.2R2text missing or illegible when filed :400H.sub.2O 110° C. Dynamic 6 days Amorphous V#4 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13R2.sup.2:800H.sub.2O 140° C. Dynamic 8 days Amorphous V#5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:5R2text missing or illegible when filed :400H.sub.2O 120° C. Static 6 days Amorphous V#6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5R2text missing or illegible when filed :400H.sub.2O 130° C. Static 3 days Amorphous V#7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:45R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic 8 days Amorphous V#8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:7Na.sub.2O:11R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic 6 days Amorphous V#9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:15R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic 2 days Amorphous V#10 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:20Cs.sub.2O:10R2.sup.4:800H.sub.2O 180 Dynamic 0.2 day Amorphous V#11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R2.sup.4:500H.sub.2O 120° C. Static 3 days Amorphous V#12 150SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :15K.sub.2O:20R2.sup.4:1500H.sub.2O 160° C. Dynamic 0.5 day Amorphous V#13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R2.sup.5:500H.sub.2O 100° C. Static 8 days Amorphous V#14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25R2.sup.5:2000H.sub.2O 120° C. Dynamic 5 days Amorphous V#15 150SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:35R2.sup.5:2800H.sub.2O 120° C. Dynamic 5 days Amorphous V#16 80SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2.sup.5:1500H.sub.2O 110° C. Dynamic 5 days Amorphous V#17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:23R2.sup.6:1800H.sub.2O 115° C. Dynamic 5 days Amorphous V#18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15R2.sup.6:1100H.sub.2O 130° C. Dynamic 3 days Amorphous V#19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9R2.sup.6:800H.sub.2O 120° C. Static 8 days Amorphous V#20 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:5R2text missing or illegible when filed :150H.sub.2O 90° C. Static 15 days Amorphous V#21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5R2.sup.7:200H.sub.2O 140° C. Static 5 days Amorphous V#22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8R2.sup.8:400H.sub.2O 110° C. Static 5 days Amorphous V#23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2text missing or illegible when filed :800H.sub.2O 120° C. Dynamic 3 days Amorphous V#24 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2.sup.9:400H.sub.2O 140° C. Dynamic 5 days Amorphous V#25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2.sup.9:280H.sub.2O 110° C. Dynamic 4 days Amorphous V#26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic 5 days Amorphous V#27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic 8 days Amorphous V#28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:15R2.sup.11:1500H.sub.2O 120° C. Dynamic 4 days Amorphous V#29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic 5 days Amorphous V#30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :14Na.sub.2O:25R2text missing or illegible when filed :2500H.sub.2O 120° C. Dynamic 3 days Amorphous Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum 2-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel: R2.sup.1: Tetrapropylammonium hydroxide R2.sup.2: Triethylhexylammonium hydroxide R2.sup.3: Triethylbenzylammonium hydroxide R2.sup.4: N,N,N-tripropyl adamantylammonium hydroxide R2.sup.5: Dipropyldibutylammonium hydroxide R2.sup.6: Benzyltripropylammonium hydroxide R2.sup.7: Choline R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Tributyl-hydroxyethyl ammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00003 TABLE 3 Types of raw materials, molar ratio thereof, addition amount of seed crystal, crystallization conditions, and crystal structure, silica- alumina ratio, and constitution of samples X1-X30 Addition amount Crystal- Crystal- silica- of seed lization lization Crystal alumina Sample Initial gel constitution crystal temperature time structure ratio constitution X1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:2.0Na.sub.2O:4.8R.sup.1:360H.sub.2O 10% 130° C. Dynamic FAU 12 0.07Na•0.07R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3.6R.sup.1:200H.sub.2O 10% 130° C. Static FAU 9 0.09Na•0.09R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 4 days X3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:5.2R.sup.1:400H.sub.2O 12% 110° C. Dynamic FAU 11 0.07K•0.08R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13R.sup.2:800H.sub.2O  8% 140° C. Dynamic FAU 15 0.03Na•0.07R.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:5R.sup.2:400H.sub.2O 15% 120° C. Static FAU 8 0.08Na•0.12R.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5R.sup.1:400H.sub.2O 10% 130° C. Static FAU 11 0.07Na•0.08Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:45R2text missing or illegible when filed :6000H.sub.2O 12% 120° C. Dynamic FAU 28 0.02Na•0.05Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:7Na.sub.2O:11R.sup.1:800H.sub.2O  8% 140° C. Dynamic FAU 18 0.03Na•0.07Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:15R.sup.1:900H.sub.2O  9% 140° C. Dynamic FAU 20 0.03Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X10 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:4R.sup.4:200H.sub.2O  5% 120° C. Static FAU 9 0.018R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R.sup.4:500H.sub.2O 14% 120° C. Static FAU 13 0.07Na•0.06R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 10 days X12 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :2.5Na.sub.2O:5R.sup.4:400H.sub.2O 16% 120° C. Static FAU 10 0.09Na•0.08R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 12 days X13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R2text missing or illegible when filed :500H.sub.2O 20% 100° C. Static FAU 13 0.09Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25R2text missing or illegible when filed :2000H.sub.2O 16% 120° C. Dynamic FAU 20 0.04Na•0.05Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:35R2text missing or illegible when filed :2800H.sub.2O 17% 120° C. Dynamic FAU 25 0.03Na•0.04Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2text missing or illegible when filed :1500H.sub.2O 10% 110° C. Dynamic FAU 18 0.04Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Cs2O:23Rtext missing or illegible when filed :1800H.sub.2O  9% 115° C. Dynamic FAU 20 0.03Cs•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15Rtext missing or illegible when filed :1100H.sub.2O  7% 130° C. Dynamic FAU 15 0.06Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9Rtext missing or illegible when filed :800H.sub.2O 13% 120° C. Static FAU 14 0.06Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X20 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:5Rtext missing or illegible when filed :150H.sub.2O 16% 90° C. Static FAU 7 0.13Na•0.09Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 15 days X21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5Rtext missing or illegible when filed :200H.sub.2O 10% 140° C. Static FAU 8 0.11Na•0.09Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8R.sup.8:400H.sub.2O 12% 110° C. Static FAU 12 0.09Na•0.05Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R.sup.8:800H.sub.2O 12% 160° C. Dynamic FAU 20 0.03Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 1 day X24 20SiO.sub.2.sup.3:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R.sup.9:400H.sub.2O 15% 140° C. Dynamic FAU 12 0.08Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:3.0Na.sub.2O:4R.sup.9:280H.sub.2O 10% 110° C. Dynamic FAU 10 0.09Na•0.08Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:10Na.sub.2O:18R.sup.10:2000H.sub.2O 12% 120° C. Dynamic FAU 20 0.04Na•0.05R.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R.sup.10:2800H.sub.2O 11% 120° C. Dynamic FAU 30 0.02Na•0.04R.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R1.sup.1:1500H.sub.2O 10% 120° C. Dynamic FAU 16 0.04Na•0.07R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 7 days X29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R1.sup.1:1500H.sub.2O  9% 120° C. Dynamic FAU 12 0.06Na•0.08R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R1.sup.1:2500H.sub.2O 10% 180° C. Dynamic FAU 25 0.02Na•0.05R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 0.5 day Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.4: N-ethyl-3-butylpyridine R.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.6: 1,4-dipropylpiperazine R.sup.7: N-methylpyridine R.sup.8: N-ethyl-3-butylpyridine R.sup.9: 1-ethyl-3-butylimidazole hydroxide R.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00004 TABLE 4 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples V1-V30 Crystallization Crystallization Crystal Sample Initial gel constitution temperature manner and time structure V1 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:4.8Rtext missing or illegible when filed :360H.sub.2O 130° C. Dynamic 5 days Amorphous V2 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3.6Rtext missing or illegible when filed :200H.sub.2O 130° C. Static 4 days Amorphous V3 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1.8K.sub.2O:5.2Rtext missing or illegible when filed :400H.sub.2O 110° C. Dynamic 6 days Amorphous V4 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13Rtext missing or illegible when filed :800H.sub.2O 140° C. Dynamic 8 days Amorphous V5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:5Rtext missing or illegible when filed :400H.sub.2O 120° C. Static 6 days Amorphous V6 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5Rtext missing or illegible when filed :400H.sub.2O 130° C. Static 3 days Amorphous V7 200SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :25Na.sub.2O:45Rtext missing or illegible when filed :6000H.sub.2O 120° C. Dynamic 8 days Amorphous V8 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:11Rtext missing or illegible when filed :800H.sub.2O 140° C. Dynamic 6 days Amorphous V9 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:15R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic 6 days Amorphous V10 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4R.sup.4:200H.sub.2O 120° C. Static 8 days Amorphous V11 30SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7Rtext missing or illegible when filed :500H.sub.2O 120° C. Static 10 days Amorphous V12 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2.5Na.sub.2O:5Rtext missing or illegible when filed :400H.sub.2O 120° C. Static 12 days Amorphous V13 30SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7Rtext missing or illegible when filed :500H.sub.2O 100° C. Static 8 days Amorphous V14 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25Rtext missing or illegible when filed :2000H.sub.2O 120° C. Dynamic 5 days Amorphous V15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:35Rtext missing or illegible when filed :2800H.sub.2O 120° C. Dynamic 5 days Amorphous V16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18Rtext missing or illegible when filed :1500H.sub.2O 110° C. Dynamic 5 days Amorphous V17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Cs.sub.2O:23Rtext missing or illegible when filed :1800H.sub.2O 115° C. Dynamic 5 days Amorphous V18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15Rtext missing or illegible when filed :1100H.sub.2O 130° C. Dynamic 3 days Amorphous V19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9Rtext missing or illegible when filed :800H.sub.2O 120° C. Static 8 days Amorphous V20 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:1.5Rtext missing or illegible when filed :150H.sub.2O 90° C. Static 15 days Amorphous V21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5Rtext missing or illegible when filed :200H.sub.2O 140° C. Static 5 days Amorphous V22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8Rtext missing or illegible when filed :400H.sub.2O 110° C. Static 5 days Amorphous V23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12Rtext missing or illegible when filed :800H.sub.2O 160° C. Dynamic 1 day Amorphous V24 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4Rtext missing or illegible when filed :400H.sub.2O 140° C. Dynamic 3 days Amorphous V25 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4Rtext missing or illegible when filed :280H.sub.2O 110° C. Dynamic 5 days Amorphous V26 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18Rtext missing or illegible when filed :2000H.sub.2O 120° C. Dynamic 5 days Amorphous V27 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:30Rtext missing or illegible when filed :2800H.sub.2O 120° C. Dynamic 8 days Amorphous V28 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R1.sup.1:1500H.sub.2O 120° C. Dynamic 7 days Amorphous V29 40SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R1.sup.1:1500H.sub.2O 120° C. Dynamic 5 days Amorphous V30 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :14Na.sub.2O:25Rtext missing or illegible when filed :2500H.sub.2O 180° C. Dynamic 0.5 day Amorphous Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.4: N-ethyl-3-butylpyridine R.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.6: 1,4-dipropylpiperazine R.sup.7: N-methylpyridine R.sup.8: N-ethyl-3-butylpyridine R.sup.9: 1-ethyl-3-butylimidazole hydroxide R.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

Example 4 Preparation of Sample X1

[0278] Preparation of synthetic gel: 0.7 g sodium aluminate (Al.sub.2O.sub.3:48.3 wt %, Na.sub.2O: 36.3 wt %, China National Pharmaceutical (Group) Shanghai Chemical Reagent Company), 0.20 g sodium hydroxide, 13.74 g N,N-dimethyl-3,5-dipropylpiperidine hydroxide (25 wt %.) were dissolved in 1.82 g deionized water and stirred until to be clear. 13.3 g silica sol (SiO.sub.2:30 wt % Shenyang Chemical Co., Ltd.) was added therein dropwise and stirred for 2 hours. Then 0.4 g Y zeolite as seed crystal with silica-alumina ratio of 3 was added, and stirring was continued for 2 hours.

[0279] Synthesis at high-silica Y zeolite: The synthesis gel was transferred into a stainless-steel reactor, and was subject to rotational crystallization at 130° C. for 5 days. After the crystallization was completed, the obtained solid was separated from liquid, washed to be neutrality, then dried at 100° C. for 12 hours. The obtained sample was denoted as sample X1.

[0280] X-ray diffraction (XRD) spectrum of sample X1 is shown in FIG. 5. demonstrating that the sample X1 is molecular sieve having FAU framework structure. Scanning electron microscope (SEM) image thereof is shown in FIG. 6, demonstrating that the particles of sample X1 are small pieces with a size ranging from 50 nm to 200 nm. .sup.29Si MAS NMR spectrum thereof is shown in FIG. 7. The fitting calculation shows that the silica-alumina ratio in the framework is consistent with the calculation results conducted by XRF. According to the XRF and .sup.13C MAS NMR normalization analysis, the element constitution of sample X1 is 0.07Na.0.07R.sup.1.(SiO.sub.0.86Al.sub.0.14)O.sub.2, where R.sup.1 is N,N-dimethyl-3,5-dipropylpiperidine hydroxide.

Example 5: Preparation of Samples

[0281] The preparation process of any one of sample X2-X30 is the same as that of Example 4. The raw materials for preparing samples X2-X30, molar ratio thereof, addition amount of seed crystal (weight ratio of seed crystal to SiO.sub.2 in gel), crystallization conditions, crystal structure, silica-alumina ratio (the silica-alumina radio of the obtained product is measured by X-ray fluorescence analyzer (XRF)) and the product constitution are shown in Table 3.

[0282] Samples X1-X20 were prepared using silica-alumina to molecular sieves having FAU topology as seed crystals, of which silica-alumina ratios were 3, 2.8, 3.5, 40, 5, 6.6, 6, 6, 7, 92, 10, 3.5, 4. 6, 8, 4. 35, 12, 20 respectively, and which were purchased from Zibo Runxin Chemical Technology Co., Ltd. Samples X21-X30 were prepared using silica-alumina molecular sieves having EMT topology as seed crystals, of which silica-alumina ratios were 7, 7, 8.5, 7, 8, 10, 21, 32.8 and 7 respectively, and which were purchased from Henan Purchased by Hnamyu Molecular Steve Co., Ltd.

Comparative Example 2: Preparation of Comparative Samples V1-V30

[0283] The preparation process of any one of samples V1-V30 is the same as that of Example 4, except that there is no seed crystal addition step. Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples V1-V30 are shown in Table 4. The samples obtained are denoted as comparative samples V1-V30.

Example 6: Characterization and Analysis of Sample X1-X30 and Comparative Samples V1-V30

[0284] The phases of sample X1-X30 and comparative samples V1-V30 were analyzed by X-ray diffraction method.

[0285] The results show that each of the samples X1-X30 prepared in Examples 4 and 5 is Y molecular sieve with both high purity and high crystallinity. The XRD spectrum of sample X1 as typical representative is shown in FIG. 5. SEM image thereof is shown in FIG. 6, and Si NWR thereof is shown in FIG. 7. The XRD spectrum result of any one of samples X2-X30 is close to FIG. 1. In other words, the diffraction peak positions and shapes are substantially identical. The relative peak intensity fluctuates within ±5% depending on the change of synthesis conditions, demonstrating that any of samples X1-X30 has the structural characteristics of Y zeolite and has no impurities. The silica-alumina ratio of any sample is much higher than that of conventional Y zeolite. It can be seen that during the synthesis of the high-silica Y molecular sieve according to the present application the introduction of nitrogen-containing heterocyclic templating agent is the key to the synthesis of the high-silica Y molecular sieve according to the present application.

[0286] In Table 4, each of the comparative samples V1-V30 is amorphous, and a XRD spectrum of the comparative sample V1 as typical representative is shown in FIG. 4. It can be seen that during the synthesis of high-silica Y zeolite, in addition to the introduction of nitrogen-containing heterocyclic templating agent, the introduction of seed crystal is also necessary.

TABLE-US-00005 TABLE 3 Types of raw materials, molar ratio thereof, addition amount of seed crystal, crystallization conditions, and crystal structure, silica- alumina ratio, and constitution of samples X1-X30 Addition amount Crystal- Crystal- silica- of seed lization lization Crystal alumina Sample Initial gel constitution crystal temperature time structure ratio constitution X1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:4.8R.sup.1:360H.sub.2O 10% 130° C. Dynamic FAU 12 0.07Na•0.07R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3.6R.sup.1:200H.sub.2O 10% 130° C. Static FAU 9 0.09Na•0.09R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 4 days X3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:5.2R.sup.1:400H.sub.2O 12% 110° C. Dynamic FAU 11 0.07K•0.08R.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13R.sup.2:800H.sub.2O  8% 140° C. Dynamic FAU 15 0.03Na•0.07R.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:5R.sup.2:400H.sub.2O 15% 120° C. Static FAU 8 0.08Na•0.12R.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5R.sup.1:400H.sub.2O 10% 130° C. Static FAU 11 0.07Na•0.08Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:45R2.sup.3:6000H.sub.2O 12% 120° C. Dynamic FAU 28 0.02Na•0.05Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:7Na.sub.2O:11R.sup.1:800H.sub.2O  8% 140° C. Dynamic FAU 18 0.03Na•0.07Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 6 days X9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:15R.sup.1:900H.sub.2O  9% 140° C. Dynamic FAU 20 0.03Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X10 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4R.sup.4:200H.sub.2O  5% 120° C. Static FAU 9 0.018R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R.sup.4:500H.sub.2O 14% 120° C. Static FAU 13 0.07Na•0.06R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 10 days X12 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :2.5Na.sub.2O:5R.sup.4:400H.sub.2O 16% 120° C. Static FAU 10 0.09Na•0.08R.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 12 days X13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R.sup.1:500H.sub.2O 20% 100° C. Static FAU 13 0.09Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25R2text missing or illegible when filed :2000H.sub.2O 16% 120° C. Dynamic FAU 20 0.04Na•0.05Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:35R2text missing or illegible when filed :2800H.sub.2O 17% 120° C. Dynamic FAU 25 0.03Na•0.04Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:18R2text missing or illegible when filed :1800H.sub.2O 10% 110° C. Dynamic FAU 18 0.04Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Cs.sub.2O:23Rtext missing or illegible when filed :1800H.sub.2O  9% 115° C. Dynamic FAU 20 0.03Cs•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15Rtext missing or illegible when filed :1100H.sub.2O  7% 130° C. Dynamic FAU 15 0.06Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9Rtext missing or illegible when filed :800H.sub.2O 13% 120° C. Static FAU 14 0.06Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X20 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:5Rtext missing or illegible when filed :150H.sub.2O 16% 90° C. Static FAU 7 0.13Na•0.09Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 15 days X21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5Rtext missing or illegible when filed :200H.sub.2O 10% 140° C. Static FAU 8 0.11Na•0.09R.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8R.sup.8:400H.sub.2O 12% 110° C. Static FAU 12 0.09Na•0.05R.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12Rtext missing or illegible when filed :800H.sub.2O 12% 160° C. Dynamic FAU 20 0.03Na•0.06R.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 1 day X24 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4Rtext missing or illegible when filed :400H.sub.2O 15% 140° C. Dynamic FAU 12 0.08Na•0.06Rtext missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 3 days X25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R.sup.9:280H.sub.2O 10% 110° C. Dynamic FAU 10 0.09Na•0.08R.sup.9(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:10Na.sub.2O:18R.sup.10:2000H.sub.2O 12% 120° C. Dynamic FAU 20 0.04Na•0.05R.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R.sup.10:2800H.sub.2O 11% 120° C. Dynamic FAU 30 0.02Na•0.04R.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 8 days X28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:15R.sup.11:1500H.sub.2O 10% 120° C. Dynamic FAU 16 0.04Na•0.07R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 7 days X29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:5Na.sub.2O:10R.sup.11:1500H.sub.2O  9% 120° C. Dynamic FAU 12 0.06Na•0.08R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 5 days X30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25Rtext missing or illegible when filed :2500H.sub.2O 10% 180° C. Dynamic FAU 25 0.02Na•0.05R.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 0.5 day Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.4: N-ethyl-3-butylpyridine R.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.6: 1,4-dipropylpiperazine R.sup.7: N-methylpyridine R.sup.8: N-ethyl-3-butylpyridine R.sup.9: 1-ethyl-3-butylimidazole hydroxide R.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00006 TABLE 4 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples V1-V30 Crystallization Crystallization Crystal Sample Initial gel constitution temperature manner and time structure V1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:4.8R.sup.1:360H.sub.2O 130° C. Dynamic 5 days Amorphous V2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3.6R.sup.1:200H.sub.2O 130° C. Static 4 days Amorphous V3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:5.2R.sup.1:400H.sub.2O 110° C. Dynamic 6 days Amorphous V4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:13R.sup.2:800H.sub.2O 140° C. Dynamic 8 days Amorphous V5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:5R.sup.2:400H.sub.2O 120° C. Static 6 days Amorphous V6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:4.5R.sup.1:400H.sub.2O 130° C. Static 3 days Amorphous V7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:45R2.sup.3:6000H.sub.2O 120° C. Dynamic 8 days Amorphous V8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:7Na.sub.2O:11R.sup.1:800H.sub.2O 140° C. Dynamic 6 days Amorphous V9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:15R.sup.1:900H.sub.2O 140° C. Dynamic 6 days Amorphous V10 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4R.sup.4:200H.sub.2O 120° C. Static 8 days Amorphous V11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R.sup.4:500H.sub.2O 120° C. Static 10 days Amorphous V12 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :2.5Na.sub.2O:5R.sup.4:400H.sub.2O 120° C. Static 12 days Amorphous V13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:7R.sup.1:500H.sub.2O 100° C. Static 8 days Amorphous V14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:25R2text missing or illegible when filed :2000H.sub.2O 120° C. Dynamic 5 days Amorphous V15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:35R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic 5 days Amorphous V16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:18R2text missing or illegible when filed :1800H.sub.2O 110° C. Dynamic 5 days Amorphous V17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Cs.sub.2O:23Rtext missing or illegible when filed :1800H.sub.2O 115° C. Dynamic 5 days Amorphous V18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :7Na.sub.2O:15Rtext missing or illegible when filed :1100H.sub.2O 130° C. Dynamic 3 days Amorphous V19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:9Rtext missing or illegible when filed :800H.sub.2O 120° C. Static 8 days Amorphous V20 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:5Rtext missing or illegible when filed :150H.sub.2O 90° C. Static 15 days Amorphous V21 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:5Rtext missing or illegible when filed :200H.sub.2O 140° C. Static 5 days Amorphous V22 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4.8R.sup.8:400H.sub.2O 110° C. Static 5 days Amorphous V23 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12Rtext missing or illegible when filed :800H.sub.2O 160° C. Dynamic 1 day Amorphous V24 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4Rtext missing or illegible when filed :400H.sub.2O 140° C. Dynamic 3 days Amorphous V25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R.sup.9:280H.sub.2O 110° C. Dynamic 5 days Amorphous V26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:10Na.sub.2O:18R.sup.10:2000H.sub.2O 120° C. Dynamic 5 days Amorphous V27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R.sup.10:2800H.sub.2O 120° C. Dynamic 8 days Amorphous V28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:15R.sup.11:1500H.sub.2O 120° C. Dynamic 7 days Amorphous V29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:5Na.sub.2O:10R.sup.11:1500H.sub.2O 120° C. Dynamic 5 days Amorphous V30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25Rtext missing or illegible when filed :2500H.sub.2O 180° C. Dynamic 0.5 day Amorphous Note: Al.sub.2O.sub.3text missing or illegible when filed .sup.1: Alumina: Al.sub.2O.sub.3text missing or illegible when filed .sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3text missing or illegible when filed .sup.3: Sodium aluminate: Al.sub.2O.sub.3text missing or illegible when filed .sup.4: Aluminum nitrate: Al.sub.2O.sub.3text missing or illegible when filed .sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3text missing or illegible when filed .sup.6: Aluminum sulfate: Al.sub.2O.sub.3text missing or illegible when filed .sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.4: N-ethyl-3-butylpyridine R.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide R.sup.6: 1,4-dipropylpiperazine R.sup.7: N-methylpyridine R.sup.8: N-ethyl-3-butylpyridine R.sup.9: 1-ethyl-3-butylimidazole hydroxide R.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

Example 7: Preparation of Sample Y #1

[0287] Preparation of directing agent 1.3 g sodium hydroxide (analytical purity, Tianjin Koenion Chemical Reagent Co., Ltd.) and 1.7 g alumina (chemical purity, China National Pharmaceutical (Group) Shanghai Chemical Reagent Co., Ltd.) were dissolved in 84.1 g tetraethylammonium hydroxide (35 wt % aqueous solution, Aladdin reagent (Shanghai) Co., Ltd.) and stirred until to be clear. 34.7 g ethyl orthosilicate was added therein dropwise (chemical purity. China pharmaceutical (Group) Shanghai chemical reagent company) and stirred for 2 hours. The obtained solution was allowed to stand at 50° C. for 12 hours to perform aging, and then stand at 100° C. for 45 hours.

[0288] Preparation of synthetic gel: 0.7 g sodium aluminate (Al.sub.2O.sub.3: 48.3 wt %, Na.sub.2O: 34.3 wt %, China National Pharmaceutical (Grow) Shanghai Chemical Reagent Company), 0.20 g sodium hydroxide, and 9.8 g tetrapropylammonium hydroxide (25 wt %) were dissolved in 4.8 g deionized water and stirred until to be clear. 13.3 g silica sol (SiO.sub.2: 30 wt %, Shenyang Chemical Co., Ltd.) was added therein dropwise and stirred far 2 hours. Then 4.9 g the above-mentioned directing agent was added therein and stirred for 3 hours.

[0289] Synthesis of high-silica Y molecular sieve: The synthetic gel was transferred into a stainless-steel reactor, and was subject to rotational crystallization at 130° C. for 5 days. After the crystallization was completed, the obtained solid was separated from liquid, washed to be neutrality, then dried at 100° C. for 12 hours. The obtained sample was denoted as sample Y #1.

[0290] X-ray diffraction (XRD) spectrum of sample Y #1 is shown in FIG. 9. demonstrating that the sample Y #1 is molecular sieve having FAU framework structure. Scanning electron microscope (SEM) image thereof is shown in FIG. 10. demonstrating that the particles of sample Y #1 are small pieces with a size ranging from 50 nm to 200 nm. .sup.29Si MAS NMR spectrum thereof is shown in FIG. 11. The fitting calculation shows that the silica-alumina ratio in the framework is consistent with the calculation results conducted by XRF. According to the XRF and .sup.13C MAS NMR normalization analysis, the element constitution of sample Y #1 is 0.07Na.0.02R1.sup.2.0.05R2.sup.1 (Si.sub.0.85Al.sub.0.14)O.sub.2, where R1.sup.2 is tetraethylammonium hydroxide, R2.sup.1 is tetrapropylammonium hydroxide.

Example 8: Preparation of Samples Y #2-Y #30

[0291] The preparation process of any one of samples Y #2-Y #30 is the same as that of Example 7. The raw materials for preparing samples Y #2-Y #30, molar ratio thereof, crystallization conditions, crystal structure, and silica-alumina ratio (the silica-alumina ratio of the obtained product is measured by X-ray fluorescence analyzer (XRF)) are shown in Table 5. Aging temperature and time for preparing directing agent, aging manner, addition amount of directing agent and sample constitution are shown in Table 6.

TABLE-US-00007 TABLE 5 Types of raw materials, molar ratio thereof, crystallization conditions, crystal structure, and silica-alumina ratio of samples Y#1-Y#30 Silica- Crystal- Crystal- alumina lization lization Crystal ratio of Sample Directing agent constitution Initial gel constitution temperature time structure product Y#1 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:12R1.sup.2:180H.sub.2O 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:2.0Na.sub.2O:3.6R2.sup.1:360H.sub.2O 130° C. Dynamic FAU 12 5 days Y#2 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:10R1.sup.1:180H.sub.2O 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3R2.sup.1:200H.sub.2O 130° C. Static FAU 9 4 days Y#3 30SiO.sub.2:1Al.sub.2O.sub.3.sup.4:1.5K2O:30R1.sup.1:600H.sub.2O 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8K2O:4R2.sup.1:400H.sub.2O 110° C. Dynamic FAU 11 6 days Y#4 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:10R1.sup.1:8R1.sup.1:400H.sub.2O 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:8.0Na.sub.2O:9R2.sup.2:800H.sub.2O 160° C. Dynamic FAU 15 3 days Y#5 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:10R1.sup.1:200H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:4.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static FAU 8 6 days Y#6 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:14R1.sup.2:200H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 130° C. Static FAU 11 3 days Y#7 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.1:1Cs2O:10R1.sup.1:180H.sub.2O 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Cs2O:40R2.sup.1:3000H.sub.2O 120° C. Dynamic FAU 28 8 days Y#8 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.5Na.sub.2O:35R1.sup.2:600H.sub.2O 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic FAU 18 6 days Y#9 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.0Na.sub.2O:34R1.sup.4:600H.sub.2O 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic FAU 20 6 days Y#10 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1.sup.1:180H.sub.2O 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.4:200H.sub.2O 120° C. Static FAU 9 8 days Y#11 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.4:500H.sub.2O 120° C. Static FAU 13 10 days Y#12 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1.sup.1:180H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.4:400H.sub.2O 120° C. Static FAU 10 12 days Y#13 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2text missing or illegible when filed :500H.sub.2O 100° C. Static FAU 13 8 days Y#14 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1.sup.1:200H.sub.2O 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2text missing or illegible when filed :2000H.sub.2O 120° C. Dynamic FAU 20 5 days Y#15 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:8R1.sup.4:100H.sub.2O 150SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:28R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic FAU 25 5 days Y#16 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:15R1.sup.1:250H.sub.2O 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:15R2text missing or illegible when filed :1500H.sub.2O 110° C. Dynamic FAU 18 5 days Y#17 30SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:20R1.sup.1:600H.sub.2O 100SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.6:180H.sub.2O 115° C. Dynamic FAU 20 5 days Y#18 5SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1.sup.1:100H.sub.2O 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2.sup.6:1100H.sub.2O 130° C. Dynamic FAU 15 8 days Y#19 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:10R1.sup.1:100H.sub.2O 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static FAU 14 8 days Y#20 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.4:5Na.sub.2O:18R1.sup.1:400H.sub.2O 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:0.1Na.sub.2O:4R2.sup.7:150H.sub.2O 90° C. Static FAU 7 15 days Y#21 10SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:8R1text missing or illegible when filed :200H.sub.2O 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:3R2.sup.7:200H.sub.2O 140° C. Static FAU 8 5 days Y#22 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:12R1text missing or illegible when filed :280H.sub.2O 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.8:400H.sub.2O 110° C. Static FAU 12 5 days Y#23 12SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:10R1.sup.4:200H.sub.2O 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 120° C. Dynamic FAU 20 6 days Y#24 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:18R1text missing or illegible when filed :400H.sub.2O 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2.sup.9:400H.sub.2O 140° C. Dynamic FAU 12 5 days Y#25 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1text missing or illegible when filed :400H.sub.2O 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2text missing or illegible when filed :280H.sub.2O 110° C. Dynamic FAU 10 5 days Y#26 8SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8R1.sup.1:150H.sub.2O 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic FAU 20 5 days Y#27 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:7R1text missing or illegible when filed :180H.sub.2O 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic FAU 30 8 days Y#28 9SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1text missing or illegible when filed :150H.sub.2O 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.11:1500H.sub.2O 120° C. Dynamic FAU 16 7 days Y#29 25SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:8R1.sup.2:480H.sub.2O 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2text missing or illegible when filed :1500H.sub.2O 120° C. Dynamic FAU 12 5 days Y#30 30SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:40R1text missing or illegible when filed :600H.sub.2O 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R2.sup.11:2500H.sub.2O 180° C. Dynamic FAU 25 3 days Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum 2-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel: R1.sup.1: Tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: Tetrapropylammonium hydroxide R2.sup.2: Triethylhexylammonium hydroxide R2.sup.3: Triethylbenzylammonium hydroxide R2.sup.4: N,N,N-tripropylamacrylammonium hydroxide: R2.sup.5: Dipropyldibutyl ammonium hydroxide R2.sup.6: Benzyltriporpylammonium hydroxide R2.sup.7: Choline: R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Butyl-hydroxyethylammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00008 TABLE 6 Aging temperature and time for preparing directing agent, addition amount of directing agent and sample constitution of samples Y#1-Y#30 Addition amount of Aging time for preparing directing Sample directing agent agent Sample constitution Y#1 40° C. 5 days + 60° C. 4 days  8% 0.07Na0.02R1.sup.20.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#2 120° C. 1 day 15% 0.09Na0.04R1text missing or illegible when filed 0.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#3 40° C. 1 day + 80° C. 4 days 10% 0.07K0.03R1text missing or illegible when filed 0.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#4 100° C. 2 days 10% 0.03Na0.04R1text missing or illegible when filed 0.05R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#5 90° C. 3 days 20% 0.08Na0.04R1text missing or illegible when filed 0.08R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#6 80° C. 5 days 10% 0.07Na0.04R1text missing or illegible when filed 0.06R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#7 40° C. 0.5 day + 80° C. 2 days  5% 0.02Cs0.01R1text missing or illegible when filed 0.04R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#8 40° C. 0.5 day + 60° C. 2 days  8% 0.03Na0.04R1text missing or illegible when filed 0.04R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#9 30° C. 3 days + 100° C. 2 days 10% 0.03Na0.02R1text missing or illegible when filed 0.04R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#10 30° C. 3 days + 50° C. 8 days 12% 0.09Na0.04R1text missing or illegible when filed 0.05R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#11 40° C. 15 days  1% 0.07Na0.02R1text missing or illegible when filed 0.04R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#12 30° C. 25 days  5% 0.09Na0.02R1text missing or illegible when filed 0.06R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#13 100° C. 5 days 15% 0.09Na0.02R1text missing or illegible when filed 0.05R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#14 80° C. 7 days  2% 0.04Na0.01R1text missing or illegible when filed 0.04R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#15 110° C. 1.5 days 18% 0.03Na0.01R1.sup.30.03R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#16 90° C. 3 days 18% 0.04Na0.02R1text missing or illegible when filed 0.04R2text missing or illegible when filed (Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#17 80° C. 5 days 18% 0.03Na0.02R1text missing or illegible when filed 0.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#18 60° C. 8 days  8% 0.06Na0.02R1text missing or illegible when filed 0.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#19 40° C. 11 days 11% 0.06Na0.02R1.sup.40.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#20 80° C. 7 days  3% 0.13Na0.04R1text missing or illegible when filed 0.05R2.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#21 80° C. 7 days 10% 0.11Na0.04R1text missing or illegible when filed 0.05R2.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#22 100° C. 5 days 10% 0.09Na0.02R1text missing or illegible when filed 0.03R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#23 110° C. 2 days 10% 0.03Na0.02R1.sup.40.04R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#24 70° C. 7 days 18% 0.08Na0.01R1text missing or illegible when filed 0.05R2.sup.9(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#25 80° C. 5 days  8% 0.09Na0.04R1text missing or illegible when filed 0.04R2.sup.9(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#26 60° C. 8 days  9% 0.04Na0.02R1text missing or illegible when filed 0.03R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#27 120° C. 1 day 20% 0.02Na0.01R1text missing or illegible when filed 0.03R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#28 110° C. 3 days 10% 0.04Na0.04R1text missing or illegible when filed 0.03R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#29 110° C. 3 days 10% 0.06Na0.03R1text missing or illegible when filed 0.05R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y#30 80° C. 7 days 10% 0.02Na0.01R1text missing or illegible when filed 0.04R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Note: R1.sup.1: tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: tetrapropylammonium hydroxide R2.sup.2: Triethyl-hexylammonium hydroxide R2.sup.3: Triethylbenzylammonium hydroxide R2.sup.4: N,N,N-tripropyladamantylammonium hydroxide: R2.sup.5: Dipropyl-dibutylammonium hydroxide: R2.sup.6: Triporpyl-benzylammonium hydroxide R2.sup.7: Choline R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Tributyl-hydroxyethyl ammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

Comparative Example 3: Preparation of Comparative Samples S #1-S #30

[0292] The specific types of raw materials for preparing synthetic gel, molar ratio thereof, preparation process and crystallization conditions are the same as those in the preparation of sample Y #1 in Example 7. There is no directing agent preparation step, and there is not addition of directing agent in the subsequent gel synthesis step. The type of raw materials, molar ratio thereof, crystallization conditions, and crystal structures of product are shown in Table 7. The obtained samples are denoted as comparative samples S #1-S #30.

TABLE-US-00009 TABLE 7 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples S#1-S#30 Crystallization Crystallization Product Sample Initial gel constitution temperature time structure S#1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.3:2.0Na.sub.2O:3.6R2.sup.1:360H.sub.2O 130° C. Dynamic 5 days Amorphous S#2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3R2.sup.1:200H.sub.2O 130° C. Static 4 days Amorphous S#3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8K.sub.2O:4R2.sup.1:400H.sub.2O 110° C. Dynamic 6 days Amorphous S#4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:9R2.sup.2:800H.sub.2O 150° C. Dynamic 3 days Amorphous S#5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static 6 days Amorphous S#6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 130° C. Static 3 days Amorphous S#7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Cs.sub.2O:40R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic 8 days Amorphous S#8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic 6 days Amorphous S#9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic 6 days Amorphous S#10 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2text missing or illegible when filed :200H.sub.2O 120° C. Static 8 days Amorphous S#11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2text missing or illegible when filed :500H.sub.2O 120° C. Static 10 days Amorphous S#12 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2text missing or illegible when filed :400H.sub.2O 120° C. Static 12 days Amorphous S#13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2text missing or illegible when filed :500H.sub.2O 100° C. Static 8 days Amorphous S#14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2text missing or illegible when filed :2000H.sub.2O 120° C. Dynamic 5 days Amorphous S#15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:28R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic 5 days Amorphous S#16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2text missing or illegible when filed :1500H.sub.2O 110° C. Dynamic 5 days Amorphous S#17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.6:1800H.sub.2O 115° C. Dynamic 5 days Amorphous S#18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2.sup.6:1100H.sub.2O 130° C. Dynamic 8 days Amorphous S#19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static 8 days Amorphous S#20 10SiO.sub.2.sup.3:1Al.sub.2O.sub.3.sup.2:0.1Na.sub.2O:4R2.sup.7:150H.sub.2O 90° C. Static 15 days Amorphous S#21 15SiO.sub.2.sup.3:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:3R2.sup.7:200H.sub.2O 140° C. Static 5 days Amorphous S#22 20SiO.sub.2.sup.3:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2.sup.8:400H.sub.2O 110° C. Static 5 days Amorphous S#23 50SiO.sub.2.sup.3:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 120° C. Dynamic 6 days Amorphous S#24 20SiO.sub.2.sup.3:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2.sup.9:400H.sub.2O 140° C. Dynamic 5 days Amorphous S#25 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:3.0Na.sub.2O:4R2.sup.9:280H.sub.2O 110° C. Dynamic 5 days Amorphous S#26 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic 5 days Amorphous S#27 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic 8 days Amorphous S#28 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:15R2.sup.11:1500H.sub.2O 120° C. Dynamic 7 days Amorphous S#29 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic 5 days Amorphous S#30 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R2.sup.11:2500H.sub.2O 180° C. Dynamic 3 days Amorphous Note: Al.sub.2O.sub.3.sup.1: alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum 2-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: fumed silica: SiO.sub.2.sup.4: Silica gel: R2.sup.1: tetrapropylammonium hydroxide: R2.sup.2: Triethyl-hexylammonium hydroxide: R2.sup.3: triethyl-benzylammonium hydroxide: R2.sup.4: N,N,N-tripropyladamantylammonium hydroxide: R2.sup.5: Dipropyldibutyl ammonium hydroxide: R2.sup.6: Benzyltriporpylammonium hydroxide R2.sup.7: Choline R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Tributyl-hydroxyethyl ammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

Comparative Example 4: Preparation of Comparative Samples T #1-T #30

[0293] The specific types of raw materials, molar ratio thereof, preparation process and crystallization conditions are the same as those of sample Y #1 in Example 7, except that after the batching step of the directing agent is completed, only stirring at room temperature for 2 hours without aging was performed. The types of raw materials, molar ratio thereof, crystallization conditions, addition amount of directing agent, and the crystal structure of the prepared product are shown in Table 8. The obtained samples were denoted a comparative samples T #1-T #30.

TABLE-US-00010 TABLE 8 Types of raw materials, addition amount of directing agent, molar ratio thereof, crystallization conditions, and crystal structure of samples T#1-T#30 Addition amount of Crystal- Crystal- Sam- directing lization lization Crystal ple Directing agent constitution agent Initial gel constitution temperature time structure T#1 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:12R1.sup.2:180H.sub.2O  8% 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:2.0Na.sub.2O:3.6R2.sup.1:360H.sub.2O 130° C. Dynamic Amorphous 5 days T#2 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 15% 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3R2.sup.1:200H.sub.2O 130° C. Static Amorphous 4 days T#3 30SiO.sub.2:1Al.sub.2O.sub.3text missing or illegible when filed :1.5K2O:30R1.sup.1:600H.sub.2O 10% 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8K2O:4R2.sup.1:400H.sub.2O 110° C. Dynamic Amorphous 6 days T#4 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:10R1text missing or illegible when filed :8R1.sup.1:400H.sub.2O 10% 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:9R2.sup.2:800H.sub.2O 160° C. Dynamic Amorphous 3 days T#5 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:10R1text missing or illegible when filed :200H.sub.2O 20% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static Amorphous 6 days T#6 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:10R1.sup.2:200H.sub.2O 10% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :40020H.sub.2O 130° C. Static Amorphous 3 days T#7 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.1:1Cs2O:10R1text missing or illegible when filed :180H.sub.2O  5% 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Cs2O:40R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic Amorphous 8 days T#8 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.5Na.sub.2O:35R1.sup.2:600H.sub.2O  8% 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic Amorphous 6 days T#9 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.0Na.sub.2O:34R1.sup.4:600H.sub.2O 10% 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic Amorphous 6 days T#10 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O 12% 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.4:200H.sub.2O 120° C. Static Amorphous 8 days T#11 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O  1% 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.4:500H.sub.2O 120° C. Static Amorphous 10 days T#12 15SiO.sub.2.sup.3:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O  5% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.4:400H.sub.2O 120° C. Static Amorphous 12 days T#13 10SiO.sub.2.sup.3:1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 15% 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.3:500H.sub.2O 100° C. Static Amorphous 8 days T#14 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :200H.sub.2O  2% 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.1:12Na.sub.2O:20R2text missing or illegible when filed :2000H.sub.2O 120° C. Dynamic Amorphous 5 days T#15 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:8R1text missing or illegible when filed :100H.sub.2O 18% 150SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:28R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic Amorphous 5 days T#16 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:15R1.sup.1:250H.sub.2O 18% 80SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:15R2text missing or illegible when filed :1500H.sub.2O 110° C. Dynamic Amorphous 5 days T#17 30SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :20R1.sup.1:600H.sub.2O 18% 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.6:1800H.sub.2O 115° C. Dynamic Amorphous 5 days T#18 5SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1.sup.1:100H.sub.2O  8% 60SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:5Na.sub.2O:12R2text missing or illegible when filed :1100H.sub.2O 130° C. Dynamic Amorphous 8 days T#19 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:12R1.sup.4:180H.sub.2O 11% 45SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static Amorphous 8 days T#20 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.4:5Na.sub.2O:18R1.sup.1:400H.sub.2O  3% 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.1Na.sub.2O:4R2.sup.7:150H.sub.2O 90° C. Static Amorphous 15 days T#21 10SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:8R1.sup.1:200H.sub.2O 10% 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:3R2.sup.7:200H.sub.2O 140° C. Static Amorphous 5 days T#22 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:12R1text missing or illegible when filed :280H.sub.2O 10% 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2.sup.8:400H.sub.2O 110° C. Static Amorphous 5 days T#23 12SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:10R1.sup.4:200H.sub.2O 10% 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 120° C. Dynamic Amorphous 5 days T#24 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:18R1.sup.1:400H.sub.2O 18% 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 140° C. Dynamic Amorphous 5 days T#25 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1.sup.1:400H.sub.2O  8% 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2.sup.9:280H.sub.2O 110° C. Dynamic Amorphous 5 days T#26 8SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8R1.sup.1:150H.sub.2O  9% 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic Amorphous 5 days T#27 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:7R1.sup.1:180H.sub.2O 20% 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic Amorphous 8 days T#28 9SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.6:0.5Na.sub.2O:8R1text missing or illegible when filed :150H.sub.2O 10% 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.11:1500H.sub.2O 120° C. Dynamic Amorphous 7 days T#29 25SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:1Na.sub.2O:8R1.sup.2:480H.sub.2O 10% 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic Amorphous 5 days T#30 30SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:3Na.sub.2O:40R1.sup.1:600H.sub.2O 10% 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R2.sup.11:2500H.sub.2O 180° C. Dynamic Amorphous 3 days Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum 2-butoxide. Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel: R1.sup.1: Tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: Tetrapropylammonium hydroxide: R2.sup.2: Triethylhexylammonium hydroxide: R2.sup.3: Triethylbenzylammonium hydroxide: R2.sup.4: N,N,N-tripropylamacrylammonium hydroxide R2.sup.5: Dipropyldibutyl ammonium hydroxide: R2.sup.6: Benzyltriporpylammonium hydroxide R2.sup.7: Choline: R2.sup.8: Tetrabutylammonium hydroxide R2.sup.9: Tetrahexylammonium hydroxide R2.sup.10: Tributyl-hydroxyethyl ammonium hydroxide R2.sup.11: Tripropyl-hydroxyethylammonium hydroxide text missing or illegible when filed indicates data missing or illegible when filed

Example 9: Characterization and Analysis of Samples Y #1-Y #30 and Comparative Samples S #1 and T #1

[0294] The phase of samples Y #1-Y #30 and comparative samples S #1-S #30 and T #1-T #30 were analyzed by X-ray diffraction method.

[0295] The result show that the each of samples Y #1-Y #30 prepared in Examples 7 and 8 is Y molecular sieve with both high purity and high crystallinity. The XRD spectrum of sample Y #1 as typical representative is shown in FIG. 9. SEM image thereof is shown in FIG. 10, and Si NMR thereof is shown in FIG. 11. The XRD spectrum result of any one of samples Y #2-Y #30 is close to FIG. 9. In other words, the diffraction peak positions and shapes are substantially identical. The relative peak intensity fluctuates within ±5% depending on the change of synthesis conditions, demonstrating that any of samples Y #1-Y #30 has the structural characteristics of Y zeolite and has no impurities.

[0296] The comparative samples S #1-S #30 and the comparative samples T #1-T #30 in Table 7 and Table 8 am amorphous. The XRD spectra of the comparative sample S #1 and the comparative sample T #1 are shown in FIGS. 12 and 13, respectively. It can be seen that, during the synthesis of high-silica Y molecular sieve, the addition of a directing agent is necessary, and high-temperature aging must be carried out during preparation of the directing agent to induce crystallization, which is the key to the synthesis of high-silica Y molecular sieve.

Example 10 Preparation of Sample Y1

[0297] Preparation of directing agent: 1.3 g sodium hydroxide (analytical parity, Tianjin Kocniou Chemical Reagent Co., Ltd.) and 1.7 g alumina (chemical purity. China National Pharmaceutical (Group) Shanghai Chemical Reagent Co., Ltd.) were dissolved in 84.1 g tetraethylammonium hydroxide (35 wt % aqueous solution, Aladdin reagent (Shanghai) Co., Ltd.) and stirred until to be clear. 34.7 g ethyl orthosilicate was added therein dropwise (chemical purity. China pharmaceutical (Group) Shanghai chemical reagent company) and stirred for 2 hours. The obtained solution was allowed to stand at 50° C. for 12 hours to perform aging and then to stand at 70° C. for 2 days.

[0298] Preparation of synthetic gel: 0.7 g sodium aluminate (Al.sub.2O.sub.3: 48.3 wt %, Na.sub.2O: 36.3 wt %, China National Pharmaceutical (Group) Shanghai Chemical Reagan Company), 0.20 g sodium hydroxide, and 10.30 g N,N-dimethyl-3,5-dipropylpiperidine hydroxide (25 wt %) were dissolved in 4.4 g deionized water and stirred until to be clear. 13.3 g silica sol (SiO.sub.2: 30 wt %, Shenyang Chemical Co., Ltd.) was added thereof dropwise and stirred for 2 hours. Then 4.9 g the above-motored directing agent was added therein and stirred for 3 hours.

[0299] Synthesis of high-silica Y molecular sieve: The synthetic gel was transferred into a stainless-steel reactor, was placed at 120° C. for 5 days under autogenous pressure. Then the obtained solid was separated from liquid, washed to be neutrality, and dried at 100° C. for 12 hours. The obtained sample was denoted as sale Y1.

[0300] X-ray diffraction (XRD) spectrum of sample Y1 is shown in FIG. 14, demonstrating that the sample Y1 is molecular sieve having FAU framework structure. Scanning electron microscope (SEM) image thereof is shown in FIG. 15. demonstrating that the particles of sample Y1 are small pieces with a size ranging from 50 nm to 200 nm. .sup.29Si MAS NMR spectrum thereof is shown in FIG. 16. The fitting calculation shows that the silica-alumina ratio in the framework is consistent with the calculations results conducted by XRF. According to the XRF and .sup.13C MAS NMR normalization analysis, the element constitution of sample Y1 is 0.07Na.0.02R1.sup.2.0.05R2.sup.1 (Si.sub.0.85Al.sub.0.14)O.sub.2, wherein, R1.sup.2 is a tetraethylammonium hydroxide, R2.sup.1 is N,N-dimethyl-3,5-dipropyl-piperidine hydroxide.

Example 11: Preparation of Samples Y2-Y30

[0301] The preparation process of any one of samples Y2-Y30 is the same as that of Example 10. The raw materials for preparing samples Y2-Y30, molar ratio thereof, crystallization conditions, crystal structure, and silica-alumina ratio (the silica-alumina ratio of the obtained product is measured by X-ray fluorescence analyzer (XRF) are shown in Table 3. Aging temperature and time for preparing directing agent, addition amount of directing agent and sample constitution are shown in Table 10.

Comparative Example 5: Preparation of Comparative Samples S1-S30

[0302] The specific preparation process is the same as that in the preparation of sample Y1 in Example 10, except that there is no directing agent preparation step, and there is not addition of directing agent in the subsequent gel synthesis step. The types of raw materials, molar ratio thereof, crystallization conditions and product structure of the prepared products are shown in Table 11. The samples obtained are denoted as comparative samples S1-S30.

Comparative Example 6: Preparation of Comparative Samples T1-T30

[0303] The specific preparation process is the same as that m to preparation of sample Y1 in Example 10, except that after the batching step of the directing agent is completed, only stirring at room temperature for 2 hours without aging was performed. Types of raw materials, molar ratio thereof, crystallization conditions, addition amount of directing agent and product structure of each synthesized product are shown in Table 12. The samples obtained are denoted as comparative samples T1-T30.

Example 12: Characterization and Analysis of Samples Y1-Y30 and Comparative Samples S1-S30 and T1-T30

[0304] The phases of samples Y1-Y30 and comparative samples S1-S30 and T1-T30 were analyzed by X-my diffraction method.

[0305] The results show that each of samples Y1-Y30 prepared in Examples 10 and 11 is Y molecular sieve with both high purity and high crystallinity. The XRD spectrum of sample Y1 as typical representative is shown in FIG. 14. SEM image thereof is shown in FIG. 15, and Si NMR thereof is shown in FIG. 16. The XRD spectrum result of my one of samples Y2-Y30 is close to FIG. 14. In other words, the diffraction peak positions and shapes are substantially identical. The relative peak intensity fluctuates within ±5% depending on the change of synthesis conditions, demonstrating that any of samples Y1-Y30 has the structural characteristics of Y zeolite and has no impurities.

[0306] In tables 9 and 10, the comparative samples S1-S30 and the comparative samples T1-T30 are all amorphous. As a typical representative, the XRD spectra of the comparative sample S1 and the comparative sample T1 are shown in FIG. 17 and FIG. 18, respectively. It can be seen that during the synthesis of high-silica Y molecular sieve, the addition of a directing agent is necessary, and high-temperature aging must be carried out during preparation of the directing agent to induce crystallization, which is the key to the synthesis of high-silica Y molecular sieve.

TABLE-US-00011 TABLE 9 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples Y1-Y30 Crystal- Crys- Crystal- lization tal Silica- Sam- lization manner/ struc- Alumina ple Directing agent constitution Initial gel constitution temperature time ture ratio Y1 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:12R1.sup.2:180H.sub.2O 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:2.0Na.sub.2O:3.6R2.sup.1:360H.sub.2O 130° C. Dynamic FAU 12 5 days Y2 10SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:10R1.sup.1:180H.sub.2O 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3R2.sup.1:200H.sub.2O 130° C. Static FAU 9 4 days Y3 30SiO.sub.2:1Al.sub.2O.sub.3.sup.4:1.5Na.sub.2O:30R1.sup.1:600H.sub.2O 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.1:400H.sub.2O 110° C. Dynamic FAU 11 6 days Y4 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:10R1.sup.1:8R1.sup.1:400H.sub.2O 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:9R2.sup.2:800H.sub.2O 140° C. Dynamic FAU 15 8 days Y5 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:10R1.sup.1:200H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static FAU 8 6 days Y6 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:14R1.sup.2:200H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 130° C. Static FAU 11 3 days Y7 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:40R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic FAU 29 8 days Y8 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.5Na.sub.2O:35R1.sup.2:600H.sub.2O 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic FAU 19 6 days Y9 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.0Na.sub.2O:34R1.sup.4:600H.sub.2O 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic FAU 20 6 days Y10 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.4:200H.sub.2O 120° C. Static FAU 9 8 days Y11 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.4:500H.sub.2O 120° C. Static FAU 13 10 days Y12 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.4:400H.sub.2O 120° C. Static FAU 10 12 days Y13 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2text missing or illegible when filed :500H.sub.2O 100° C. Static FAU 13 8 days Y14 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :200H.sub.2O 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2text missing or illegible when filed :2000H.sub.2O 120° C. Dynamic FAU 20 5 days Y15 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:8R1text missing or illegible when filed :100H.sub.2O 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:28R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic FAU 25 5 days Y16 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15R1text missing or illegible when filed :150H.sub.2O 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:15R2text missing or illegible when filed :1500H.sub.2O 110° C. Dynamic FAU 18 5 days Y17 30SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :20R1text missing or illegible when filed :600H.sub.2O 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2text missing or illegible when filed :1800H.sub.2O 115° C. Dynamic FAU 20 5 days Y18 5SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :100H.sub.2O 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2#Z,899.sup.6:1100H.sub.2O 130° C. Dynastic FAU 15 8 days Y19 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1.sup.4:180H.sub.2O 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static FAU 14 8 days Y20 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.4:0.5Na.sub.2O:18R1text missing or illegible when filed :400H.sub.2O 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:0.1Na.sub.2O:4R2.sup.7:150H.sub.2O 90° C. Static FAU 7 15 days Y21 10SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:8R1text missing or illegible when filed :200H.sub.2O 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:3R2.sup.7:200H.sub.2O 140° C. Static FAU 8 5 days Y22 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:12R1text missing or illegible when filed :280H.sub.2O 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2.sup.8:400H.sub.2O 110° C. Static FAU 12 5 days Y23 12SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:10R1.sup.4:200H.sub.2O 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 120° C. Dynamic FAU 20 6 days Y24 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:18R1text missing or illegible when filed :400H.sub.2O 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2.sup.9:400H.sub.2O 140° C. Dynamic FAU 12 5 days Y25 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1text missing or illegible when filed :400H.sub.2O 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2.sup.9:280H.sub.2O 110° C. Dynamic FAU 10 5 days Y26 8SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8R1text missing or illegible when filed :150H.sub.2O 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic FAU 20 5 days Y27 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:7R1text missing or illegible when filed :180H.sub.2O 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic FAU 30 8 days Y28 9SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.6:0.5Na.sub.2O:8R1text missing or illegible when filed :150H.sub.2O 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R21.sup.1:1500H.sub.2O 120° C. Dynamic FAU 16 7 days Y29 25SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:1Na.sub.2O:8R1.sup.2:180H.sub.2O 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic FAU 12 5 days Y30 30SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.6:3Na.sub.2O:40R1text missing or illegible when filed :600H.sub.2O 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R2.sup.11:2500H.sub.2O 120° C. Dynamic FAU 25 6 days Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel: R1.sup.1: Tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide: R2.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide: R2.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide: R2.sup.4: N-ethyl-3-butylpyridine R2.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide: R2.sup.6: 1,4-dipropylpiperazine R2.sup.7: N-methylpyridine. R2.sup.8: N-ethyl-3-butylpyridine R2.sup.9: 1-ethyl-3-butylimidazole hydroxide R2.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R2.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00012 TABLE 10 Aging temperature and time for preparing directing agent, addition amount of directing agent and sample constitution of samples Y1-Y30 Addition amount of Aging time for preparing directing Sample directing agent agent Sample constitution Y1 40° C. 5 days + 60° C. 4 days  8% 0.07Na0.02R1.sup.20.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y2 120° C. 1 day 15% 0.09Na0.04R1text missing or illegible when filed 0.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y3 40° C. 1 day + 80° C. 4 days 10% 0.07K0.03R1text missing or illegible when filed 0.05R2.sup.1(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y4 100° C. 2 days 10% 0.03Na0.04R1text missing or illegible when filed 0.05R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y5 90° C. 3 days 20% 0.08Na0.04R1text missing or illegible when filed 0.08R2.sup.2(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y6 80° C. 5 days 10% 0.07Na0.05R1.sup.20.06R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y7 40° C. 0.5 day + 80° C. 2 days  5% 0.02Na0.01R1text missing or illegible when filed 0.04R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y8 40° C. 0.5 day + 60° C. 2 days  8% 0.03Na0.04R1.sup.20.04R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y9 30° C. 3 days + 100° C. 2 days 10% 0.03Na0.02R1.sup.40.04R2.sup.3(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y10 30° C. 3 days + 50° C. 8 days 12% 0.09Na0.04R1text missing or illegible when filed 0.05R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y11 40° C. 15 days  7% 0.07Na0.02R1text missing or illegible when filed 0.04R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y12 30° C. 25 days  5% 0.09Na0.02R1text missing or illegible when filed 0.06R2.sup.4(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y13 100° C. 5 days 15% 0.09Na0.02R1text missing or illegible when filed 0.05R2.sup.5(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y14 80° C. 7 days 10% 0.04Na0.01R1text missing or illegible when filed 0.04R2.sup.5(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y15 110° C. 1.5 days 18% 0.03Na0.01R1text missing or illegible when filed 0.03R2.sup.5(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y16 90° C. 3 days 18% 0.04Na0.02R1text missing or illegible when filed 0.04R2.sup.5(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y17 80° C. 5 days 18% 0.03Na0.02R1text missing or illegible when filed 0.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y18 60° C. 8 days  8% 0.06Na0.02R1text missing or illegible when filed 0.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y19 40° C. 11 days 11% 0.06Na0.02R1text missing or illegible when filed 0.04R2.sup.6(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y20 80° C. 7 days  5% 0.13Na0.04R1text missing or illegible when filed 0.05R2.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y21 80° C. 7 days 10% 0.11Na0.04R1text missing or illegible when filed 0.05R2.sup.7(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y22 100° C. 5 days 10% 0.09Na0.02R1text missing or illegible when filed 0.03R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y23 110° C. 2 days 10% 0.03Na0.02R1text missing or illegible when filed 0.04R2.sup.8(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y24 70° C. 7 days 18% 0.08Na0.01R1text missing or illegible when filed 0.05R2.sup.9(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y25 80° C. 5 days  8% 0.09Na0.04R1text missing or illegible when filed 0.04R2.sup.9(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y26 60° C. 8 days  9% 0.04Na0.02R1text missing or illegible when filed 0.03R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y27 120° C. 1 day 20% 0.02Na0.01R1text missing or illegible when filed 0.03R2.sup.10(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y28 110° C. 3 days 10% 0.04Na0.04R1text missing or illegible when filed 0.03R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y29 110° C. 3 days 10% 0.06Na0.03R1text missing or illegible when filed 0.05R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Y30 80° C. 7 days 10% 0.02Na0.01R1text missing or illegible when filed 0.04R2.sup.11(Sitext missing or illegible when filed Altext missing or illegible when filed )O.sub.2 Note: R1.sup.1: tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R2.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R2.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R2.sup.4: N-ethyl-3-butylpyridine: R2.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide: R2.sup.6: 1,4-dipropylpiperazine R2.sup.7: N-methylpyridine R2.sup.8: N-ethyl-3-butylpyridine R2.sup.9: 1-ethyl-3-butylimidazole hydroxide R2.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R2.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00013 TABLE 11 Types of raw materials, molar ratio thereof, crystallization conditions, and crystal structure of samples S1-S30 Crystallization Crystallization Product Sample Initial gel constitution temperature time structure S1 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :2.0Na.sub.2O:3.6R2text missing or illegible when filed :360H.sub.2O 130° C. Dynamic 5 days Amorphous S2 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3R2text missing or illegible when filed :200H.sub.2O 130° C. Static 4 days Amorphous S3 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 110° C. Dynamic 6 days Amorphous S4 50SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:9R2.sup.2:800H.sub.2O 140° C. Dynamic 8 days Amorphous S5 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static 6 days Amorphous S6 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 130° C. Static 3 days Amorphous S7 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:40R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic 8 days Amorphous S8 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic 6 days Amorphous S9 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic 6 days Amorphous S10 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2.sup.4:200H.sub.2O 120° C. Static 8 days Amorphous S11 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.4:500H.sub.2O 120° C. Static 10 days Amorphous S12 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.4:400H.sub.2O 120° C. Static 12 days Amorphous S13 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.5:500H.sub.2O 120° C. Static 8 days Amorphous S14 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.5:2000H.sub.2O 100° C. Dynamic 5 days Amorphous S15 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:28R2.sup.5:2800H.sub.2O 120° C. Dynamic 5 days Amorphous S16 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.5:1500H.sub.2O 110° C. Dynamic 5 days Amorphous S17 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.6:1800H.sub.2O 115° C. Dynamic 5 days Amorphous S18 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2.sup.6:1100H.sub.2O 130° C. Dynamic 8 days Amorphous S19 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static 8 days Amorphous S20 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3R2.sup.7:200H.sub.2O 90° C. Static 15 days Amorphous S21 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 140° C. Static 5 days Amorphous S22 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 110° C. Static 5 days Amorphous S23 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 120° C. Dynamic 6 days Amorphous S24 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2.sup.9:280H.sub.2O 140° C. Dynamic 5 days Amorphous S25 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:18R2.sup.10:2000H.sub.2O 110° C. Dynamic 5 days Amorphous S26 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic 5 days Amorphous S27 80SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.10:1500H.sub.2O 120° C. Dynamic 8 days Amorphous S28 40SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic 7 days Amorphous S29 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :14Na.sub.2O:25R2.sup.11:2500H.sub.2O 120° C. Dynamic 5 days Amorphous S30 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:3R2text missing or illegible when filed :200H.sub.2O 120° C. Dynamic 6 days Amorphous Note: Al.sub.2O.sub.3.sup.1: alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: fumed silica: SiO.sub.2.sup.4: Silica gel: R2.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide: R2.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide: R2.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide: R2.sup.4: N-ethyl-3-butylpyridine: R2.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide: R2.sup.6: 1,4-dipropylpiperazine R2.sup.7: N-methylpyridine: R2.sup.8: N-ethyl-3-butylpyridine R2.sup.9: 1-ethyl-3-butylimidazole hydroxide R2.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R2.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

TABLE-US-00014 TABLE 11 Types of raw materials, addition amount of directing agent, molar ratio thereof, crystallization conditions, and product structure of samples T1-T30 addition Crystal- amount Crystal- lization Sam- of seed lization manner/ Product ple Directing agent constitution crystal Initial gel constitution temperature time structure T1 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:12R1.sup.2:180H.sub.2O  8% 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:2.0Na.sub.2O:3.6R2.sup.1:360H.sub.2O 130° C. Dynamic Amorphous 5 days T2 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.1:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 15% 15SiO.sub.2.sup.1:1Al.sub.2O.sub.3.sup.1:1.8Na.sub.2O:3R2text missing or illegible when filed :200H.sub.2O 130° C. Static Amorphous 4 days T3 30SiO.sub.2:1Al.sub.2O.sub.3.sup.1:1.5Na.sub.2O:30R1.sup.1:600H.sub.2O 10% 20SiO.sub.2.sup.1:1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2.sup.2:400H.sub.2O 110° C. Dynamic Amorphous 6 days T4 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10R1text missing or illegible when filed :8R1text missing or illegible when filed :400H.sub.2O 10% 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8.0Na.sub.2O:9R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic Amorphous 8 days T5 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:10R1text missing or illegible when filed :200H.sub.2O 20% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:3.0Na.sub.2O:4R2.sup.2:400H.sub.2O 120° C. Static Amorphous 5 days T6 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:0.5Na.sub.2O:14R1.sup.2:200H.sub.2O 10% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 130° C. Static Amorphous 3 days T7 10SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O  5% 200SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:25Na.sub.2O:40R2text missing or illegible when filed :3000H.sub.2O 120° C. Dynamic Amorphous 8 days T8 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.5Na.sub.2O:35R1.sup.2:600H.sub.2O  8% 50SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:8.0Na.sub.2O:6R2text missing or illegible when filed :800H.sub.2O 140° C. Dynamic Amorphous 6 days T9 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.4:1.0Na.sub.2O:34R1.sup.4:600H.sub.2O 10% 60SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:9.0Na.sub.2O:8R2text missing or illegible when filed :900H.sub.2O 140° C. Dynamic Amorphous 6 days T10 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O 12% 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:4R2.sup.4:200H.sub.2O 120° C. Static Amorphous 8 days T11 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O  7% 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2.sup.4:500H.sub.2O 120° C. Static Amorphous 10 days T12 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1text missing or illegible when filed :180H.sub.2O  5% 20SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:5R2.sup.4:400H.sub.2O 120° C. Static Amorphous 12 days T13 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1Na.sub.2O:10R1text missing or illegible when filed :180H.sub.2O 15% 30SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :5.0Na.sub.2O:6R2text missing or illegible when filed :500H.sub.2O 120° C. Static Amorphous 8 days T14 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :200H.sub.2O 10% 100SiO.sub.2.sup.2:1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2text missing or illegible when filed :2000H.sub.2O 100° C. Dynamic Amorphous 5 days T15 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:8R1text missing or illegible when filed :100H.sub.2O 18% 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15Na.sub.2O:25R2text missing or illegible when filed :2800H.sub.2O 120° C. Dynamic Amorphous 5 days T16 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:15R1text missing or illegible when filed :250H.sub.2O 18% 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:10Na.sub.2O:15R2text missing or illegible when filed :1500H.sub.2O 110° C. Dynamic Amorphous 5 days T17 30SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :R:600H.sub.2O 18% 100SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :12Na.sub.2O:20R2.sup.6:1800H.sub.2O 115° C. Dynamic Amorphous 5 days T18 5SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:10R1text missing or illegible when filed :100H.sub.2O  8% 60SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:12R2text missing or illegible when filed :1100H.sub.2O 130° C. Dynamic Amorphous 8 days T19 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:12R1.sup.4:180H.sub.2O 11% 45SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :4Na.sub.2O:8R2.sup.6:800H.sub.2O 120° C. Static Amorphous 8 days T20 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.4:0.5Na.sub.2O:18R1text missing or illegible when filed :400H.sub.2O  5% 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:0.1Na.sub.2O:4R2text missing or illegible when filed :150H.sub.2O 90° C. Static Amorphous 15 days T21 10SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1text missing or illegible when filed :200H.sub.2O 10% 15SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.2:1.8Na.sub.2O:3R2text missing or illegible when filed :200H.sub.2O 140° C. Static Amorphous 5 days T22 15SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:12R1text missing or illegible when filed :280H.sub.2O 10% 20SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :1.8Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 110° C. Static Amorphous 5 days T23 12SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.7:0.5Na.sub.2O:10R1.sup.4:200H.sub.2O 10% 50SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:8R2.sup.8:800H.sub.2O 120° C. Dynamic Amorphous 6 days T24 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:18R1text missing or illegible when filed :400H.sub.2O 18% 20SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :4.0Na.sub.2O:4R2text missing or illegible when filed :400H.sub.2O 140° C. Dynamic Amorphous 5 days T25 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :0.5Na.sub.2O:8R1text missing or illegible when filed :400H.sub.2O  8% 15SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3.0Na.sub.2O:4R2text missing or illegible when filed :280H.sub.2O 110° C. Dynamic Amorphous 5 days T26 8SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :8R1text missing or illegible when filed :150H.sub.2O  9% 100SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:10Na.sub.2O:18R2.sup.10:2000H.sub.2O 120° C. Dynamic Amorphous 5 days T27 10SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :2Na.sub.2O:7R1text missing or illegible when filed :180H.sub.2O 20% 150SiO.sub.2.sup.4:1Al.sub.2O.sub.3.sup.7:15Na.sub.2O:30R2.sup.10:2800H.sub.2O 120° C. Dynamic Amorphous 8 days T2B 9SiO.sub.2.sup.2:1Al.sub.2O.sub.3.sup.6:0.5Na.sub.2O:8R1text missing or illegible when filed :150H.sub.2O 10% 80SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :10Na.sub.2O:15R2.sup.11:1500H.sub.2O 120° C. Dynamic Amorphous 7 days T29 25SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :1Na.sub.2O:8R1text missing or illegible when filed :480H.sub.2O 10% 40SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3text missing or illegible when filed :5Na.sub.2O:10R2.sup.11:1500H.sub.2O 120° C. Dynamic Amorphous 5 days T30 30SiO.sub.2.sup.4:1Al.sub.2O.sub.3text missing or illegible when filed :3Na.sub.2O:40R1text missing or illegible when filed :600H.sub.2O 10% 150SiO.sub.2text missing or illegible when filed :1Al.sub.2O.sub.3.sup.7:14Na.sub.2O:25R2.sup.11:2500H.sub.2O 120° C. Dynamic Amorphous 6 days Note: Al.sub.2O.sub.3.sup.1: Alumina: Al.sub.2O.sub.3.sup.2: Aluminum isopropoxide: Al.sub.2O.sub.3.sup.3: Sodium aluminate: Al.sub.2O.sub.3.sup.4: Aluminum nitrate: Al.sub.2O.sub.3.sup.5: Aluminum tri-sec-butoxide: Al.sub.2O.sub.3.sup.6: Aluminum sulfate: Al.sub.2O.sub.3.sup.7: Aluminum powder: SiO.sub.2.sup.1: Silica sol: SiO.sub.2.sup.2: Ethyl orthosilicate: SiO.sub.2.sup.3: Fumed silica: SiO.sub.2.sup.4: Silica gel R1.sup.1: Tetramethylammonium hydroxide: R1.sup.2: Tetraethylammonium hydroxide: R1.sup.3: Tetrapropylammonium hydroxide: R1.sup.4: Choline: R2.sup.1: N,N-dimethyl-3,5-dipropylpiperidine hydroxide R2.sup.2: N,N-diethyl-2,6-dimethylpiperidine hydroxide R2.sup.3: N,N-diethyl-3,5-dipropylpiperidine hydroxide R2.sup.4: N-ethyl-3-butylpyridine R2.sup.5: N,N-diethyl-3,5-dipropylpiperidine hydroxide R2.sup.6: 1,4-dipropylpiperazine R2.sup.7: N-methylpyridine R2.sup.8: N-ethyl-3-butylpyridine R2.sup.9: 1-ethyl-3-butylimidazole hydroxide R2.sup.10: 1-ethyl-4-gutyl-5-methylpiperazine R2.sup.11: 1-ethyl-3-butyl-4-propylimidazole hydroxide text missing or illegible when filed indicates data missing or illegible when filed

[0307] The above example are only illustrative, and do not limit the present application in any form. Any change or modification made by the skilled in the art based on the technical content disclosed above, without departing from the spirit of the present application is equivalent example and falls within the scope of the present application.