Process for the synthesis of IZM-2 zeolite in the presence of a template, 1,6-bis(methylpiperidinium)hexane dibromide
10875778 ยท 2020-12-29
Assignee
Inventors
Cpc classification
B01J20/3078
PERFORMING OPERATIONS; TRANSPORTING
B01J20/3057
PERFORMING OPERATIONS; TRANSPORTING
B01J29/70
PERFORMING OPERATIONS; TRANSPORTING
B01J37/10
PERFORMING OPERATIONS; TRANSPORTING
B01J20/18
PERFORMING OPERATIONS; TRANSPORTING
International classification
B01J20/18
PERFORMING OPERATIONS; TRANSPORTING
B01J20/30
PERFORMING OPERATIONS; TRANSPORTING
B01J29/70
PERFORMING OPERATIONS; TRANSPORTING
B01J37/10
PERFORMING OPERATIONS; TRANSPORTING
Abstract
A novel process is described for the preparation of a microporous crystalline solid, known as IZM-2 microporous solid or IZM-2 zeolite. This novel process consists of carrying out the synthesis of IZM-2 zeolite by conversion/transformation of a zeolite with structure type FAU under hydrothermal conditions. In particular, said novel process consists of carrying out the synthesis of an IZM-2 zeolite starting from a zeolite with structure type FAU used as the source of silicon and aluminium and a specific organic molecule or template comprising two quaternary ammonium functions, namely 1,6-bis(methylpiperidinium)hexane dibromide.
Claims
1. A process for the preparation of an IZM-2 zeolite, comprising at least the following steps: i) mixing, in an aqueous medium, at least one zeolite with structure type FAU having a molar ratio SiO2 (fau)/Al2O3(fau) of greater than or equal to 30, at least one nitrogen-containing organic compound R, R being 1,6-bis(methylpiperidinium)hexane dibromide, and at least one alkali metal and/or alkaline-earth metal M with valency n, where n is a whole number greater than or equal to 1, optionally at least one additional source of an oxide XO.sub.2 in a manner such that the molar ratio XO.sub.2/SiO.sub.2 (FAU) is in the range 0 to 4, the mixture having the following molar composition: TABLE-US-00006 (XO.sub.2 + SiO.sub.2 (FAU))/Al.sub.2O.sub.3 (FAU) in the range 10 to 800, H.sub.2O/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 1 to 100, R/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.01 to 0.6, M.sub.2/nO/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.005 to 0.35, in which X is one or more tetravalent element(s) selected from the group formed by the following elements: silicon, germanium, and titanium, SiO.sub.2 (fau) being the quantity of SiO.sub.2 supplied by the FAU zeolite, and Al.sub.2O.sub.3 (fau) being the quantity of Al.sub.2O.sub.3 supplied by the FAU zeolite, ii) hydrothermal treatment of said mixture obtained from step i) at a temperature in the range 120 C. to 200 C. for a period in the range 1 day to 10 days, until said IZM-2 zeolite has been formed.
2. The process as claimed in claim 1, in which said zeolite with structure type FAU is Y zeolite.
3. The process as claimed in claim 1, in which the source of at least one alkali and/or alkaline-earth metal M is sodium hydroxide.
4. The process as claimed in claim 1, in which X is silicon.
5. The process as claimed in claim 1, in which the additional source of an oxide XO.sub.2 is added in the mixing step i) in a manner such that the molar ratio XO.sub.2/SiO.sub.2 (FAU) is in the range 0 to 3.
6. The process as claimed in claim 1, in which the reaction mixture obtained in step i) has the following molar composition: TABLE-US-00007 (XO.sub.2 + SiO.sub.2 (FAU))/Al.sub.2O.sub.3 (FAU) in the range 20 to 600, H.sub.2O/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 10 to 70, R/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.05 to 0.45, M.sub.2/nO/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.008 to 0.3.
7. The process as claimed in claim 6, in which the reaction mixture obtained in step i) has the following molar composition: TABLE-US-00008 (XO.sub.2 + SiO.sub.2 (FAU))/Al.sub.2O.sub.3 (FAU) in the range 25 to 450, H.sub.2O/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 15 to 55, R/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.085 to 0.4, M.sub.2/nO/(XO.sub.2 + SiO.sub.2 (FAU)) in the range 0.01 to 0.25.
8. The process as claimed in claim 1, in which the mixture of step i) also contains at least one source of a fluoride anion BF selected from fluorine salts, in which B is a cation selected from the cations NH.sub.4.sup.+, Na.sup., K.sup.+ and Li.sup.+, and hydrofluoric acid in aqueous solution.
9. The process as claimed in claim 1, in which the hydrothermal treatment of step ii) is carried out at a temperature in the range 120 C. to 195 C.
10. The process as claimed in claim 1, in which the hydrothermal treatment of step ii) is carried out for a period in the range 2 days to 9 days.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
(1)
(2) The invention will now be illustrated in the following examples, which are not in any case limiting in nature.
(3) Without further elaboration, it is believed that one skilled in the art can, using the preceding description, utilize the present invention to its fullest extent. The preceding preferred specific embodiments are, therefore, to be construed as merely illustrative, and not limitative of the remainder of the disclosure in any way whatsoever.
(4) In the foregoing and in the examples, all temperatures are set forth uncorrected in degrees Celsius and, all parts and percentages are by weight, unless otherwise indicated.
(5) The entire disclosures of all applications, patents and publications, cited herein and of corresponding French application No. 17/52.473, filed Mar. 24, 2017, are incorporated by reference herein.
Example 1: Preparation of 1,6-bis(methylpiperidinium)hexane dibromide (Template RBr.SUB.2.)
(6) 50 g of 1,6-dibromohexane (0.20 mole, 99%, Alfa Aesar) was added to a 1 L flask containing 50 g of N-methylpiperidine (0.51 mole, 99%, Alfa Aesar) and 200 mL of ethanol. The reaction medium was stirred and heated under reflux for 5 h. The mixture was then cooled to ambient temperature and filtered. The mixture was poured into 300 mL of cold diethylether, then the precipitate formed was filtered and washed with 100 mL of diethylether. The solid obtained was recrystallized from an ethanol/ether mixture. The solid obtained was dried under vacuum for 12 h. 71 g of a white solid was obtained (i.e. a yield of 80%).
(7) The product had the expected .sup.1H NMR spectrum. .sup.1H NMR (D.sub.2O, ppm/TMS): 1.27 (4H, m); 1.48 (4H, m); 1.61 (4H, m); 1.70 (8H, m); 2.85 (6H, s); 3.16 (12H, m).
Example 2: Preparation of an IZM-2 Solid in Accordance with the Invention
(8) 316 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3=80, Zeolyst) was mixed with 7121.7 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 3583 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 1270 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 116 mg of IZM-2 zeolite seeds was added to the synthesized mixture and stirring was maintained for 15 minutes. Next, 2116.6 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0033 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.165 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 300. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature. The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2. The diffraction spectrum for the calcined solid IZM-2 is given in
Example 3: Preparation of an IZM-2 Solid in Accordance with the Invention
(9) 303 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3, 80, Zeolyst) was mixed with 6848 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 3682 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 925 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 112 mg of IZM-2 zeolite seeds was added to the synthesized mixture and stirring was maintained for 15 minutes. Next, 2035.4 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained. i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0033 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.125 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 300. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature. The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 4: Preparation of an IZM-2 Solid in Accordance with the Invention
(10) 1803 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3, 80, Zeolyst) was mixed with 20636.3 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 11754 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 3680 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 334 mg of IZM-2 zeolite seeds was added to the synthesized mixture and stirring was maintained for 15 minutes. Next, 3847.2 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0066 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.165 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 150. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(11) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 5: Preparation of an IZM-2 Solid in Accordance with the Invention
(12) 1803 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3=80 Zeolyst) was mixed with 20636.3 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 12467 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 2788 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 334 mg of seeds of IZM-2 zeolite was added to the synthesized mixture and stirring was maintained for 15 minutes. Next, 3847.2 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0066 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.125 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 150. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(13) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 6: Preparation of an IZM-2 Solid in Accordance with the Invention
(14) 3005 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3=80, Zeolyst) was mixed with 26916.9 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 5881 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 2439 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 300 mg of seeds of IZM-2 zeolite was added to the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0125 Al.sub.2O.sub.3: 0.25 RBr.sub.2: 0.125 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 80. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(15) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 7: Preparation of an IZM-2 Solid in Accordance with the Invention
(16) 3005 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3=80, Zeolyst) was mixed with 18055.9 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 12928 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 2439 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 300 mg of IZM-2 zeolite seeds was added to the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0125 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.125 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 80. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(17) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 8: Preparation of an IZM-2 Solid in Accordance with the Invention
(18) 781 mg of a zeolite with structure type FAU (CBV720, SiO.sub.2/Al.sub.2O.sub.3, 30, Zeolyst) was mixed with 6076.6 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 4203 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 548 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 103 mg of IZM-2 zeolite seeds was added to the synthesized mixture and stirring was maintained for 15 minutes. Next, 610.3 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.025 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.0835 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 40. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature. The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 9: Preparation of an IZM-2 Solid in Accordance with the Invention
(19) 781 mg of a zeolite with structure type FAU (CBV720, SiO.sub.2/Al.sub.2O.sub.3, 30, Zeolyst) was mixed with 6076.6 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 3985 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 821 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 103 mg of IZM-2 zeolite seeds was added to the synthesised mixture and stirring was maintained for 15 minutes. Next, 610.3 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.025 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.125 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 40. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(20) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 10: Preparation of an IZM-2 Solid in Accordance with the Invention
(21) 150 mg of a zeolite with structure type FAU (CBV720, SiO.sub.2/Al.sub.2O.sub.3, 30, Zeolyst) was mixed with 1043.3 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 742 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 94 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 18 mg of seeds of IZM-2 zeolite was added to the synthesised mixture and stirring was maintained for 15 minutes. Next, 70.4 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0278 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.0835 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 36. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature. The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 11: Preparation of an IZM-2 Solid in Accordance with the Invention
(22) 150 mg of a zeolite with structure type FAU (CBV720, SiO.sub.2/Al.sub.2O.sub.3=30, Zeolyst) was mixed with 2053.1 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. The mixture was stirred for 10 minutes. 94 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 18 mg of IZM-2 zeolite seeds was added to the synthesised mixture and stirring was maintained for 15 minutes. Next, 70.4 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture, and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0278 Al.sub.2O.sub.3: 0.33 RBr.sub.2: 0.0835 Na.sub.2O: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 36. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 6 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with deionized water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature. The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
Example 12: Preparation of an IZM-2 Solid in Accordance with the Invention
(23) 54 mg of a zeolite with structure type FAU (CBV780, SiO.sub.2/Al.sub.2O.sub.3=80, Zeolyst) was mixed with 1219.1 mg of an aqueous solution of 1,6-bis(methylpiperidinium)hexane dibromide (20.04% by weight) prepared in accordance with Example 1. 558 mg of deionized water was added to the preceding mixture; stirring of the preparation obtained was maintained for 10 minutes. 217 mg of an aqueous solution containing 20% by weight of sodium hydroxide (98% by weight, Aldrich) was added. In order to promote the formation of the crystalline solid IZM-2, 5 mg of seeds of IZM-2 zeolite was added to the synthesised mixture and stirring was maintained for 15 minutes. Next, 362.7 mg of colloidal silica (Ludox HS40, 40% by weight, Aldrich) was incorporated into the synthesised mixture. Finally, 61 mg of an aqueous solution containing 10% by weight of ammonium fluoride (Aldrich) was added to the synthesised mixture and stirring was maintained for the time necessary to evaporate the solvent until the desired concentration for the gel was obtained, i.e. the molar composition of the mixture was as follows: 1 SiO.sub.2: 0.0033 Al.sub.2O.sub.3: 0.17 RBr.sub.2: 0.165 Na.sub.2O: 0.05 NH.sub.4F: 33.33 H.sub.2O, i.e. a SiO.sub.2/Al.sub.2O.sub.3 ratio of 300. The mixture was then transferred into an autoclave following homogenization. The autoclave was closed then heated for 8 days at 170 C., with stirring. The crystalline product obtained was filtered, washed with water then dried overnight at 100 C. The solid was then introduced into a muffle furnace in which a calcining step was carried out: the calcining cycle comprised a rise in temperature to 200 C., a constant temperature stage at 200 C. maintained for 2 hours, a rise in temperature to 550 C. followed by a constant temperature stage at 550 C. maintained for 8 hours, followed by a return to ambient temperature.
(24) The calcined solid product was analysed by X ray diffraction and identified as being constituted by solid IZM-2.
(25) The preceding examples can be repeated with similar success by substituting the generically or specifically described reactants and/or operating conditions of this invention for those used in the preceding examples.
(26) From the foregoing description, one skilled in the art can easily ascertain the essential characteristics of this invention and, without departing from the spirit and scope thereof, can make various changes and modifications of the invention to adapt it to various usages and conditions.