FLUIDIZED BED DEVICE FOR COUPLING NAPHTHA AND METHANOL TO PREPARE AROMATICS AND CO-PRODUCE OLEFINS AND ITS APPLICATION METHOD

Abstract

A fluidized bed device for coupling naphtha and methanol to prepare aromatics and co-produce olefins and its application method are provided. By using the device, under the action of a catalyst, naphtha reacts with methanol to generate product gas containing aromatics and light olefins as main components. The method can efficiently and selectively convert linear and branched aliphatic hydrocarbons into aromatics, while also increasing p-xylene production through aromatic methylation reactions, with the p-xylene content in the xylene mixture exceeding 75 wt %. The fluidized bed reactor achieves increased p-xylene production by controlling the progression of cascade reactions (naphtha.fwdarw.benzene/toluene.fwdarw.p-xylene). Additionally, it utilizes the methylation reaction of benzene/toluene with methanol to provide in-situ heat for the coupled naphtha-methanol aromatization process, thereby achieving autothermal balance.

Claims

1. A fluidized bed device for coupling naphtha and methanol to prepare aromatics and co-produce olefins, comprising a naphtha and methanol coupled aromatization reactor, a regenerator, and a light hydrocarbon aromatization reactor; wherein the naphtha and methanol coupled aromatization reactor is connected to the regenerator via a first spent catalyst delivery pipe; the regenerator is connected to the naphtha and methanol coupled aromatization reactor via a regenerated catalyst delivery pipe; a naphtha and methanol coupled aromatization reactor distributor is provided in the naphtha and methanol coupled aromatization reactor; the naphtha and methanol coupled aromatization reactor distributor comprises n sub-distributors, sequentially arranged from bottom to top as the 1.sup.st sub-distributor to the n.sup.th sub-distributor, wherein 2n10; the 1.sup.st sub-distributor is configured to introduce a naphtha feedstock; the 2.sup.nd to n.sup.th sub-distributors are configured to introduce a methanol feedstock; the light hydrocarbon aromatization reactor comprises a riser reactor, and the riser reactor is connected to a bed reactor; the regenerator is connected to the riser reactor via a second regenerated catalyst slide valve; the bed reactor is connected to the regenerator via a second spent catalyst delivery pipe.

2. The fluidized bed device according to claim 1, wherein an upper part of the naphtha and methanol coupled aromatization reactor is provided with a gas-solid separation zone; the gas-solid separation zone is provided with a first product gas delivery pipe; a lower part of the naphtha and methanol coupled aromatization reactor is provided with a naphtha and methanol coupled aromatization reaction zone; a naphtha and methanol coupled aromatization reactor shell is provided with a first gas-solid separation unit, a second gas-solid separation unit, and a first gas collection chamber; the first gas collection chamber is located at a top of the gas-solid separation zone, and the first gas collection chamber is connected to the first product gas delivery pipe; gas outlets of the first gas-solid separation unit and the second gas-solid separation unit are connected to the first gas collection chamber; a catalyst outlet end of the first gas-solid separation unit is located above an opening end of an inlet pipe of a first stripper; an inlet of the second gas-solid separation unit is connected to the regenerator; a catalyst outlet end of the second gas-solid separation unit is located above the opening end of the inlet pipe of the first stripper and between the 1.sup.st and 2.sup.nd sub-distributors.

3. The fluidized bed device according to claim 2, wherein the first stripper is provided below the naphtha and methanol coupled aromatization reaction zone; the naphtha and methanol coupled aromatization reaction zone is connected to the first spent catalyst delivery pipe via the first stripper.

4. The fluidized bed device according to claim 3, wherein the first stripper is connected to the first spent catalyst delivery pipe via a first spent catalyst slide valve.

5. The fluidized bed device according to claim 2, wherein the first gas-solid separation unit employs one or more sets of gas-solid cyclone separators, each set comprises a first-stage gas-solid cyclone separator and a second-stage gas-solid cyclone separator.

6. The fluidized bed device according to claim 2, wherein the second gas-solid separation unit employs one or more sets of gas-solid cyclone separators, each set comprises a first-stage gas-solid cyclone separator and a second-stage gas-solid cyclone separator.

7. The fluidized bed device according to claim 1, wherein an upper part of the regenerator is provided with a regenerator gas-solid separation zone; the regenerator gas-solid separation zone is provided with a flue gas delivery pipe; a lower part of the regenerator is provided with a regeneration zone; the second spent catalyst delivery pipe and an outlet of the first spent catalyst delivery pipe deliver a spent catalyst into the regeneration zone; the lower part of the regenerator is provided with a regenerator distributor for introducing a regeneration gas; the regenerated catalyst delivery pipe transports a regenerated catalyst from the regeneration zone to the naphtha and methanol coupled aromatization reactor; the second regenerated catalyst slide valve delivers the regenerated catalyst to the riser reactor.

8. The fluidized bed device according to claim 7, wherein a regenerator shell is provided with a regenerator gas-solid separation unit and a regenerator gas collection chamber; the regenerator gas collection chamber is located at a top of the regenerator gas-solid separation zone; a gas outlet of the regenerator gas-solid separation unit is connected to the regenerator gas collection chamber; the regenerator gas collection chamber is connected to the flue gas delivery pipe.

9. The fluidized bed device according to claim 7, wherein a regenerator stripper is provided below the regeneration zone; the regeneration zone is connected to a first regenerated catalyst slide valve and the second regenerated catalyst slide valve via the regenerator stripper; the first regenerated catalyst slide valve is connected to the naphtha and methanol coupled aromatization reactor via the regenerated catalyst delivery pipe; the second regenerated catalyst slide valve is connected to the riser reactor.

10. (canceled)

11. The fluidized bed device according to claim 8, wherein the regenerator gas-solid separation unit employs one or more sets of gas-solid cyclone separators, each set comprises a first-stage gas-solid cyclone separator and a second-stage gas-solid cyclone separator.

12. The fluidized bed device according to claim 1, wherein an upper part of the bed reactor is provided with a bed reactor gas-solid separation zone; the bed reactor gas-solid separation zone is provided with a second product gas delivery pipe; a lower part of the bed reactor is provided with a light hydrocarbon aromatization reaction zone; a lower inner part of the light hydrocarbon aromatization reaction zone is provided with a bed reactor distributor; the bed reactor distributor is configured to introduce a bed reactor feedstock; an upper end of the riser reactor penetrates a bottom of the bed reactor and is axially inserted into the bed reactor; the second regenerated catalyst slide valve delivers a catalyst to a feedstock inlet end of the riser reactor.

13. The fluidized bed device according to claim 12, wherein the bed reactor gas-solid separation zone is provided with a third gas-solid separation unit and a second gas collection chamber; a gas outlet of the third gas-solid separation unit is connected to the second gas collection chamber; a catalyst outlet of the third gas-solid separation unit is located in the light hydrocarbon aromatization reaction zone; the second gas collection chamber is connected to the second product gas delivery pipe located outside the bed reactor; wherein the light hydrocarbon aromatization reaction zone is connected to a second stripper, and the bed reactor is connected to the second spent catalyst delivery pipe via the second stripper; wherein the second stripper is connected to the second spent catalyst delivery pipe via a second spent catalyst slide valve; wherein the third gas-solid separation unit is a gas-solid cyclone separator; the catalyst outlet of the third gas-solid separation unit is located above an outlet end of the riser reactor.

14-16. (canceled)

17. A method for coupling naphtha and methanol to prepare aromatics and co-produce olefins, wherein the fluidized bed device according to claim 1 is used; a catalyst is a metal molecular sieve bifunctional catalyst; the naphtha feedstock is introduced into the naphtha and methanol coupled aromatization reactor via the 1.sup.st sub-distributor; the methanol feedstock is introduced into the naphtha and methanol coupled aromatization reactor via the 2.sup.nd to n.sup.th sub-distributors; a riser reactor feedstock containing light alkanes is introduced into the riser reactor; a bed reactor feedstock is introduced into the bed reactor; a regeneration gas is introduced into the regenerator; the naphtha and methanol coupled aromatization reactor and the bed reactor output a product gas flow, and a spent catalyst is delivered to the regenerator via the first spent catalyst delivery pipe and the second spent catalyst delivery pipe; after the spent catalyst is regenerated by reacting with the regeneration gas in the regenerator, a regenerated catalyst is delivered to the naphtha and methanol coupled aromatization reactor and the riser reactor; the regenerator discharges a flue gas; wherein the catalyst is a metal-modified HZSM-5 zeolite molecular sieve; a metal used for a metal modification is at least one selected from the group consisting of La, Zn, Ga, Fe, Mo, and Cr; the metal modification comprises: placing an HZSM-5 zeolite molecular sieve in a metal salt solution, and carrying out an impregnation, a drying, and a calcination to obtain the metal-modified HZSM-5 zeolite molecular sieve; wherein the naphtha feedstock is at least one selected from the group consisting of coal direct liquefaction naphtha, coal indirect liquefaction naphtha, straight-run naphtha, and hydrocracking naphtha.

18-19. (canceled)

20. The method according to claim 17, wherein the naphtha feedstock further comprises unconverted naphtha separated from the product gas flow, and the unconverted naphtha comprises linear aliphatic hydrocarbons, branched aliphatic hydrocarbons, and naphthenes of C.sub.4-C.sub.12.

21. The method according to claim 17, wherein reaction conditions of a naphtha and methanol coupled aromatization reaction zone are: a gas superficial linear velocity of 0.5-2.0 m/s, a reaction temperature of 500-600 C., a reaction pressure of 100-500 kPa, and a bed density of 150-700 kg/m.sup.3.

22. The method according to claim 17, wherein a carbon content in the regenerated catalyst is 0.5 wt %; wherein the regeneration gas is at least one selected from the group consisting of oxygen, air, and oxygen-enriched air; wherein reaction conditions of a regeneration zone are: a gas superficial linear velocity of 0.5-2.0 m/s, a regeneration temperature of 600-750 C., a regeneration pressure of 100-500 kPa, and a bed density of 150-700 kg/m.sup.3.

23-24. (canceled)

25. The method according to claim 17, wherein the riser reactor feedstock further comprises water vapor, with a water vapor content of 0-80 wt %; wherein the light alkanes in the riser reactor feedstock are obtained by separation from the product gas flow; wherein reaction conditions of the riser reactor are: a gas superficial linear velocity of 3.0-10.0 m/s, a temperature of 580-700 C., a pressure of 100-500 kPa, and a bed density of 50-150 kg/m.sup.3.

26-27. (canceled)

28. The method according to claim 17, wherein the bed reactor feedstock is obtained by separation from the product gas flow; wherein the bed reactor feedstock comprises unconverted naphtha separated from the product gas flow, and the unconverted naphtha comprises linear aliphatic hydrocarbons, branched aliphatic hydrocarbons, and naphthenes of C.sub.4-C.sub.12; wherein the bed reactor feedstock comprises C.sub.3, C.sub.4, and C.sub.5 hydrocarbons.

29-31. (canceled)

32. The method according to claim 17, wherein reaction conditions of a light hydrocarbon aromatization reaction zone are: a gas superficial linear velocity of 0.5-2.0 m/s, a reaction temperature of 550-665 C., a reaction pressure of 100-500 kPa, and a bed density of 150-700 kg/m.sup.3.

33. The method according to claim 17, wherein the naphtha feedstock enters a naphtha and methanol coupled aromatization reaction zone via the 1.sup.st sub-distributor of the naphtha and methanol coupled aromatization reactor distributor, contacts the catalyst from the regenerator, and generates the product gas flow containing benzene, toluene, and xylene (BTX), light olefins, hydrogen, light alkanes, combustible gas, heavy aromatics, and unconverted naphtha; the catalyst from the regenerator enters a second gas-solid separation unit to achieve gas-solid separation; a degassed catalyst enters a space between the 1.sup.st and 2.sup.nd sub-distributors; the methanol feedstock enters the naphtha and methanol coupled aromatization reaction zone via the 2.sup.nd to n.sup.th sub-distributors of the naphtha and methanol coupled aromatization reactor distributor, reacts with the benzene and the toluene in the product gas flow to undergo methylation, generating para-xylene; the catalyst from the regenerator becomes the spent catalyst due to coking in the naphtha and methanol coupled aromatization reaction zone; the product gas flow enters a first gas-solid separation unit to remove the spent catalyst entrained in the product gas flow, then enters a first gas collection chamber, and is delivered to first downstream sections via a first product gas delivery pipe; the spent catalyst in the naphtha and methanol coupled aromatization reaction zone enters a first stripper via an opening end of an inlet pipe of the first stripper, undergoes stripping, and after the stripping, passes through a first spent catalyst slide valve and the first spent catalyst delivery pipe to enter second downstream sections; the regeneration gas is introduced into a regeneration zone of the regenerator via a regenerator distributor, contacts the spent catalyst from the naphtha and methanol coupled aromatization reactor and the spent catalyst from the light hydrocarbon aromatization reactor, and a coke on the spent catalyst reacts with the regeneration gas to generate the flue gas, converting the spent catalyst into the regenerated catalyst; the riser reactor feedstock is introduced into the riser reactor via an inlet end of the riser reactor, contacts and reacts with the regenerated catalyst from the regenerator, and the riser reactor feedstock is converted into a flow containing BTX, light olefins, H.sub.2, and other components under an action of the catalyst, then enters a lower inner part of a light hydrocarbon aromatization reaction zone in the bed reactor via an outlet end of the riser reactor; the bed reactor feedstock is introduced into the light hydrocarbon aromatization reaction zone via a bed reactor distributor, contacts the catalyst from the riser reactor, and generates a light hydrocarbon aromatization product gas containing BTX, light olefins, H.sub.2, and other components, and the catalyst becomes the spent catalyst.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

[0102] FIGURE is a schematic diagram of a device for coupling naphtha and methanol to prepare aromatics and co-produce olefins according to one embodiment of the present application.

LIST OF COMPONENTS AND REFERENCE NUMERALS

[0103] 1 naphtha and methanol coupled aromatization reactor; [0104] 1-1 naphtha and methanol coupled aromatization reactor shell; [0105] 1-2 naphtha and methanol coupled aromatization reactor distributor; [0106] 1-3 gas-solid separation unit I; [0107] 1-4 gas collection chamber I; [0108] 1-5 product gas delivery pipe I; [0109] 1-6 stripper I; [0110] 1-7 spent catalyst slide valve I; [0111] 1-8 spent catalyst delivery pipe I; [0112] 1-9 gas-solid separation unit II [0113] 1-2-1 1.sup.st sub-distributor; 1-2-2 2.sup.nd sub-distributor; 1-2-3 3.sup.rd sub-distributor. [0114] 2 regenerator; [0115] 2-1 regenerator shell; [0116] 2-2 regenerator distributor; [0117] 2-3 regenerator gas-solid separation unit; [0118] 2-4 regenerator gas collection chamber; [0119] 2-5 flue gas delivery pipe; [0120] 2-6 regenerator stripper; [0121] 2-7 regenerated catalyst slide valve I; [0122] 2-8 regenerated catalyst delivery pipe; [0123] 2-9 regenerated catalyst slide valve II. [0124] 3 light hydrocarbon aromatization reactor; [0125] 3-1 inlet end of the riser reactor; [0126] 3-2 middle section of the riser reactor; [0127] 3-3 outlet end of the riser reactor; [0128] 3-4 bed reactor shell; [0129] 3-5 bed reactor distributor; [0130] 3-6 gas-solid separation unit III; [0131] 3-7 gas collection chamber II; [0132] 3-8 product gas delivery pipe II; [0133] 3-9 stripper II; [0134] 3-10 spent catalyst slide valve II; [0135] 3-11 spent catalyst delivery pipe II.

DETAILED DESCRIPTION OF THE EMBODIMENTS

[0136] The present application will be described in detail below with reference to examples, but the present application is not limited to these examples.

[0137] The following describes possible embodiments.

[0138] The present application provides a fluidized bed device for coupling naphtha and methanol to prepare aromatics and co-produce olefins, as shown in the FIGURE. The device includes a naphtha and methanol coupled aromatization reactor 1, a regenerator 2, and a light hydrocarbon aromatization reactor 3.

[0139] The naphtha and methanol coupled aromatization reactor 1 includes: a naphtha and methanol coupled aromatization reactor shell 1-1, a naphtha and methanol coupled aromatization reactor distributor 1-2, a gas-solid separation unit I 1-3, a gas collection chamber I 1-4, a product gas delivery pipe I 1-5, a stripper I 1-6, a spent catalyst slide valve I 1-7, a spent catalyst delivery pipe I 1-8, and a gas-solid separation unit II 1-9.

[0140] The naphtha and methanol coupled aromatization reactor distributor 1-2 includes: a 1.sup.st sub-distributor 1-2-1, a 2.sup.nd sub-distributor 1-2-2, and a 3.sup.rd sub-distributor 1-2-3.

[0141] The naphtha and methanol coupled aromatization reactor shell 1-1 includes an upper naphtha and methanol coupled aromatization reactor shell and a lower naphtha and methanol coupled aromatization reactor shell. The upper naphtha and methanol coupled aromatization reactor shell encloses a gas-solid separation zone, and the lower naphtha and methanol coupled aromatization reactor shell encloses a naphtha and methanol coupled aromatization reaction zone. The naphtha and methanol coupled aromatization reactor shell is provided with an outlet of the regenerated catalyst delivery pipe 2-8.

[0142] The naphtha and methanol coupled aromatization reactor distributor 1-2 is provided in the lower part of the naphtha and methanol coupled aromatization reaction zone. The naphtha and methanol coupled aromatization reactor distributor includes three sub-distributors, which are sequentially arranged from bottom to top as the 1.sup.st sub-distributor 1-2-1 to the 3.sup.rd sub-distributor 1-2-3. The 1.sup.st sub-distributor is used for introducing naphtha feedstock. The 2.sup.nd sub-distributor to the 3rd sub-distributor are used for introducing methanol feedstock.

[0143] The naphtha and methanol coupled aromatization reactor shell 1-1 is further provided with the gas-solid separation unit I 1-3, the gas-solid separation unit II 1-9 and the gas collection chamber I 1-4. The gas collection chamber I 1-4 is located at the inner top of the naphtha and methanol coupled aromatization reactor shell. The gas outlet of the gas-solid separation unit I 1-3 is connected to the gas collection chamber I 1-4. The gas collection chamber I 1-4 is connected to the product gas delivery pipe I 1-5. The catalyst outlet end of the gas-solid separation unit I 1-3 is located above the opening end of the inlet pipe of the stripper I 1-6. The inlet of the gas-solid separation unit II 1-9 is connected to the regenerator 2. The gas outlet of the gas-solid separation unit II 1-9 is connected to the gas collection chamber I 1-4. The catalyst outlet end of the gas-solid separation unit II 1-9 is located above the opening end of the inlet pipe of the stripper I 1-6, and between the 1.sup.st sub-distributor 1-2-1 and the 2.sup.nd sub-distributor 1-2-2.

[0144] The stripper I 1-6 is provided beneath the naphtha and methanol coupled aromatization reaction zone. The inlet of the stripper I 1-6 is located inside the naphtha and methanol coupled aromatization reactor shell 1-1. The outlet of the stripper I 1-6 is located outside the naphtha and methanol coupled aromatization reactor shell 1-1 and is connected to the spent catalyst slide valve I 1-7. The opening end of the inlet of the stripper I 1-6 is located above the 1.sup.st sub-distributor 1-2-1 of the naphtha and methanol coupled aromatization reactor.

[0145] The spent catalyst slide valve I 1-7 is provided beneath the stripper I 1-6. The inlet of the spent catalyst slide valve I 1-7 is connected to the outlet of the stripper I 1-6. The outlet of the spent catalyst slide valve I 1-7 is connected to the inlet of the spent catalyst delivery pipe I 1-8. The outlet of the spent catalyst delivery pipe I 1-8 is connected to the regenerator shell 2-1.

[0146] The spent catalyst slide valve I 1-7 is used for controlling the circulation amount of spent catalyst.

[0147] In a preferred embodiment, the gas-solid separation unit I 1-3 employs one or more sets of gas-solid cyclone separators, each set including a first-stage gas-solid cyclone separator and a second-stage gas-solid cyclone separator.

[0148] In a preferred embodiment, the gas-solid separation unit II 1-9 employs one or more sets of gas-solid cyclone separators, each set including a first-stage gas-solid cyclone separator and a second-stage gas-solid cyclone separator.

[0149] The regenerator 2 includes: the regenerator shell 2-1, the regenerator distributor 2-2, the regenerator gas-solid separation unit 2-3, the regenerator gas collection chamber 2-4, the flue gas delivery pipe 2-5, the regenerator stripper 2-6, the regenerated catalyst slide valve I 2-7, the regenerated catalyst delivery pipe 2-8, and the regenerated catalyst slide valve II 2-9.

[0150] The regenerator shell 2-1 includes the regenerator upper shell and the regenerator lower shell, wherein the regenerator upper shell encloses the gas-solid separation zone, and the regenerator lower shell encloses the regeneration zone; the regenerator shell 2-1 is provided with an outlet of the spent catalyst delivery pipe I 1-8 and the outlet of the spent catalyst delivery pipe II 3-11.

[0151] The regenerator distributor 2-2 is provided at the lower part of the regeneration zone, and the regenerator distributor 2-2 is used for introducing the regeneration gas.

[0152] The regenerator shell 2-1 is also provided with a regenerator gas-solid separation unit 2-3 and a regenerator gas collection chamber 2-4; the regenerator gas collection chamber 2-4 is located at the inner top of the regenerator shell 2-1; the gas outlet of the regenerator gas-solid separation unit 2-3 is connected to the regenerator gas collection chamber 2-4; the regenerator gas collection chamber 2-4 is connected to the flue gas delivery pipe 2-5; the catalyst outlet end of the regenerator gas-solid separation unit 2-3 is located above the opening end of the inlet pipe of the regenerator stripper 2-6.

[0153] The regenerator stripper 2-6 is provided below the regeneration zone; the inlet of the regenerator stripper 2-6 is located inside the regenerator shell 2-1; the outlet of the regenerator stripper 2-6 is located outside the regenerator shell 2-1, and is connected to the regenerated catalyst slide valve I 2-7 and the regenerated catalyst slide valve II 2-9; the opening end of the inlet of the regenerator stripper 2-6 is located above the regenerator distributor 2-2.

[0154] The regenerated catalyst slide valve I 2-7 is connected to the inlet of the regenerated catalyst delivery pipe 2-8, and the outlet of the regenerated catalyst delivery pipe 2-8 is connected to the inlet of the gas-solid separation unit II 1-9.

[0155] The regenerated catalyst slide valve I 2-7 is used to control the circulation amount of the regenerated catalyst.

[0156] The regenerated catalyst slide valve II 2-9 is used to control the circulation amount of the regenerated catalyst.

[0157] In a preferred embodiment, the regenerator gas-solid separation unit 2-3 uses one or more groups of gas-solid cyclone separators, and each group of gas-solid cyclone separators includes the first-stage gas-solid cyclone separator and the second-stage gas-solid cyclone separator.

[0158] The light hydrocarbon aromatization reactor 3 includes: the inlet end of the riser reactor 3-1, the middle part of the riser reactor 3-2, the outlet end of the riser reactor 3-3, the bed reactor shell 3-4, the bed reactor distributor 3-5, the gas-solid separation unit III 3-6, the gas collection chamber II 3-7, the product gas delivery pipe II 3-8, the stripper II 3-9, the spent catalyst slide valve II 3-10, and the spent catalyst delivery pipe II 3-11.

[0159] The bed reactor shell 3-4 includes an upper shell of the bed reactor and a lower shell of the bed reactor, the upper shell of the bed reactor encloses a gas-solid separation zone, and the lower shell of the bed reactor encloses a light hydrocarbon aromatization reaction zone; the bed reactor distributor 3-5 is provided at the inner lower part of the light hydrocarbon aromatization reaction zone; the upper section of the riser reactor penetrates the bottom of the bed reactor and is axially inserted in the bed reactor; the outlet end of the riser reactor 3-3 is located at the inner lower part of the light hydrocarbon aromatization reaction zone.

[0160] The gas-solid separation zone of the bed reactor is provided with the gas-solid separation unit III 3-6 and a gas collection chamber II 3-7; the gas outlet of the gas-solid separation unit III 3-6 is connected to the gas collection chamber II 3-7; the catalyst outlet of the gas-solid separation unit III 3-6 is located in the light hydrocarbon aromatization reaction zone; the gas collection chamber II 3-7 is connected to the product gas delivery pipe II 3-8 located outside the bed reactor.

[0161] The stripper II 3-9 and the spent catalyst slide valve II 3-10 are provided outside the shell of the bed reactor; the inlet of the stripper II 3-9 is located at the lower shell of the bed reactor; the outlet of the stripper II 3-9 is connected to the inlet of the spent catalyst slide valve II 3-10, the outlet of the spent catalyst slide valve II 3-10 is connected to the inlet of the spent catalyst delivery pipe II 3-11, and the outlet of the spent catalyst delivery pipe II 3-11 is connected to the regenerator shell 2-1.

[0162] In a preferred embodiment, the gas-solid separation unit III 3-6 is a gas-solid cyclone separator; the catalyst outlet of the gas-solid separation unit III 3-6 is located above the outlet end of the riser reactor 3-3.

[0163] In a preferred embodiment, a gas collection chamber II 3-7 is provided at the inner top of the bed reactor.

[0164] In a preferred embodiment, the bed reactor distributor 3-5 is used to feed the bed reactor feedstock.

[0165] In a preferred embodiment, the inlet end of the riser reactor 3-1 is connected to the regenerated catalyst slide valve II 2-9 through a pipeline.

[0166] In a preferred embodiment, the inlet end of the riser reactor 3-1 is used to feed the catalyst and the riser reactor feedstock.

[0167] The present application provides a method for coupling naphtha and methanol to prepare aromatics and co-produce olefins, the method using any of the above-mentioned devices and a metal molecular sieve bifunctional catalyst;

[0168] Optionally, The catalyst adopts metal-modified HZSM-5 zeolite molecular sieve; the metal used for metal modification is at least one selected from the group consisting of La, Zn, Ga, Fe, Mo, and Cr; [0169] the metal modification method includes: placing the HZSM-5 zeolite molecular sieve in a metal salt solution, impregnating, drying and calcining to obtain the metal modified HZSM-5 zeolite molecular sieve.

[0170] The method includes the following steps:

[0171] Naphtha enters the naphtha and methanol coupled aromatization reaction zone through the 1.sup.st sub-distributor 1-2-1 of the naphtha and methanol coupled aromatization reactor distributor 1-2, and contacts with catalyst from the regenerator 2 to generate a product gas flow containing BTX, light olefins, hydrogen, light alkanes, combustible gas, heavy aromatics and unconverted naphtha, while the catalyst; the catalyst from the regenerator 2 enters the gas-solid separation unit II 1-9 to achieve gas-solid separation, then the degassed catalyst enters between the 1.sup.st sub-distributor 1-2-1 and the 2nd sub-distributor 1-2-2; methanol enters the naphtha and methanol coupled aromatization reaction zone through the 2.sup.nd sub-distributor 1-2-2 to the 3.sup.rd sub-distributor 1-2-3 of the naphtha and methanol coupled aromatization reactor distributor 1-2 respectively, and undergoes methylation reaction with benzene and toluene in the product gas flow to generate para-xylene; the catalyst from the regenerator 2 is converted into spent catalyst through coking in the naphtha and methanol coupled aromatization reaction zone; the product gas flow enters the gas-solid separation unit I 1-3 to remove the entrained spent catalyst, then enters the gas collection chamber I 1-4, and is delivered to downstream units through the product gas delivery pipe I 1-5; the spent catalyst in the naphtha and methanol coupled aromatization reaction zone enters the stripper I 1-6 through the opening end of the inlet pipe of the stripper I 1-6 for stripping, and after stripping, passes through the spent catalyst slide valve I 1-7 and the spent catalyst delivery pipe I 1-8 to enter the regenerator 2. [0172] passing the regenerated gas into the regeneration zone of the regenerator 2 through the regenerator distributor 2-2, and contacting with the spent catalyst, the coke on the spent catalyst reacts with the regenerated gas to generate flue gas, and at the same time, the spent catalyst is converted into the regenerated catalyst; the flue gas enters the regenerator gas-solid separation unit 2-3 to remove the regenerated catalyst carried therein, and then enters the regenerator gas collection chamber 2-4, and enters the downstream section through the flue gas delivery pipe 2-5; the regenerated catalyst passes through the regenerator stripper 2-6, the regenerated catalyst slide valve I 2-7 and the regenerated catalyst delivery pipe 2-8 in sequence to enter the naphtha and methanol coupled aromatization reactor 1; the regenerated catalyst passes through the regenerator stripper 2-6 and the regenerated catalyst slide valve II 2-9 in sequence to enter the light hydrocarbon aromatization reactor 3; [0173] feeding the riser reactor feedstock into the riser reactor through the inlet end of the riser reactor 3-1, contacting and reacting with the regenerated catalyst from the regenerator, and converting the riser reactor feedstock into a flow containing components such as BTX, light olefins and H.sub.2 under the action of the catalyst, and then entering the inner lower part of the light hydrocarbon aromatization reaction zone in the bed reactor through the outlet end of the riser reactor 3-3; feeding the bed reactor feedstock into the light hydrocarbon aromatization reaction zone through the bed reactor distributor 3-5, contacting with the catalyst from the riser reactor, and generating a light hydrocarbon aromatization product gas containing components such as BTX, light olefins and H.sub.2; the light hydrocarbon aromatization product gas enters the gas-solid separation unit III 3-6 to remove the catalyst carried therein, and then enters the gas collection chamber II 3-7, and then enters the downstream section through the product gas delivery pipe II 3-8; the catalyst in the light hydrocarbon aromatization reaction zone passes through the stripper II 3-9, the spent catalyst slide valve II 3-10 and the spent catalyst delivery pipe II 3-11 to enter the regenerator 2.

[0174] The light olefins are ethylene and propylene.

[0175] The light alkanes are ethane and propane.

[0176] The combustible gas includes methane, CO and the like.

[0177] The heavy aromatic hydrocarbons refer to aromatic hydrocarbons having 9 or more carbon atoms in the molecule.

[0178] In a preferred embodiment, the naphtha is selected from at least one of coal direct liquefaction naphtha, coal indirect liquefaction naphtha, straight run naphtha and hydrocracked naphtha.

[0179] In a preferred embodiment, the naphtha further includes unconverted naphtha separated from the product gas flow.

[0180] In a preferred embodiment, the process conditions of the naphtha and methanol coupled aromatization reaction zone are: gas superficial velocity of 0.5-2.0 m/s, reaction temperature of 500-600 C., reaction pressure of 100-500 kPa, and bed density of 150-700 kg/m.sup.3.

[0181] In a preferred embodiment, the carbon content in the regenerated catalyst is 0.5 wt %.

[0182] In a preferred embodiment, the regeneration gas is selected from at least one of oxygen, air and oxygen enriched air.

[0183] In a preferred embodiment, the process conditions in the regeneration zone are: gas superficial linear velocity is 0.5-2.0 m/s, regeneration temperature is 600-750 C., regeneration pressure is 100-500 kPa, and bed density is 150-700 kg/m.sup.3.

[0184] In a preferred embodiment, the riser reactor feedstock includes water vapor and light alkanes separated from the product gas flow.

[0185] In a preferred embodiment, the water vapor content in the riser reactor feed is 0-80 wt %.

[0186] In a preferred embodiment, the process conditions of the riser reactor are: gas superficial velocity of 3.0-10.0 m/s, temperature of 580-700 C., pressure of 100-500 kPa, and bed density of 50-150 kg/m.sup.3.

[0187] In a preferred embodiment, the bed reactor feedstock includes unconverted naphtha separated from the product gas flow, with the main components of the unconverted naphtha being linear aliphatic hydrocarbons, branched aliphatic hydrocarbons and naphthenes of C.sub.4-C.sub.12.

[0188] In a preferred embodiment, the bed reactor feedstock includes C.sub.3, C.sub.4 and C.sub.5 hydrocarbons.

[0189] In a preferred embodiment, the bed reactor feedstock includes C.sub.4 and C.sub.5 hydrocarbons.

[0190] In a preferred embodiment, the C.sub.3, C.sub.4 and C.sub.5 hydrocarbons are derived from C.sub.3, C.sub.4 and C.sub.5 hydrocarbons separated from the product gas flow.

[0191] In a preferred embodiment, the C.sub.4 and C.sub.5 hydrocarbons are derived from C.sub.4 and C.sub.5 hydrocarbons separated from the product gas flow.

[0192] The C.sub.3, C.sub.4 and C.sub.5 hydrocarbons refer to hydrocarbons with 3, 4 and 5 carbon atoms.

[0193] The C.sub.4 and C.sub.5 hydrocarbons refer to hydrocarbons with 4 and 5 carbon atoms.

[0194] In the embodiment described in the present application, the naphtha feedstock has a latent aromatic content of 0-80 wt %, the single-pass conversion rate of naphtha is 70-95 wt % and the single-pass conversion rate of methanol is about 100 wt %, the unconverted naphtha is separated from the product gas and returned to the naphtha and methanol coupled aromatization reactor 1 as a raw material, some light alkanes are separated from the product gas and returned to the riser reactor in the light hydrocarbon aromatization reactor 3 as a raw material, C.sub.3, C.sub.4 and C.sub.5 hydrocarbons are separated from the product gas and returned to the bed reactor in the light hydrocarbon aromatization reactor 3 as a raw material, and the final product distribution is: 60-72 wt % BTX, 8-15 wt % light olefins, 3-7 wt % hydrogen, 3-7 wt % light alkanes, 4-6 wt % combustible gas, 4-8 wt % heavy aromatics, and 0.5-1 wt % coke. The content of p-xylene in the mixed xylene in the product is 60-75 wt %.

[0195] The catalyst used in the following Examples was prepared as follows:

[0196] 100 g of HZSM-5 zeolite molecular sieve (manufactured by Nankai University Catalyst Plant, Si/Al=15) was immersed in a 10 wt % zinc nitrate aqueous solution. The mass ratio of HZSM-5 zeolite to the zinc nitrate solution (solid-to-liquid ratio) was 1:10. The mixture was impregnated at 80 C. for 6 hours, filtered, dried at 120 C. under air atmosphere for 4 hours, and then calcined at 550 C. under air atmosphere for 4 hours to obtain a [Zn]HZSM-5 molecular sieve sample.

[0197] 100 g of the [Zn]HZSM-5 molecular sieve sample was mixed with an amorphous binder containing aluminum or silicon. Detailed steps:

[0198] The [Zn]HZSM-5 sample, pseudo-boehmite, silica sol, xanthan gum (bio-gum), and water were uniformly mixed. The mixture underwent slurrying, homogenization, and deaeration to form a slurry. The weight fractions of the slurry components were:

TABLE-US-00001 [Zn]HZSM-5 35 parts by weight Al.sub.2O.sub.3 20 parts by weight SiO.sub.2 45 parts by weight H.sub.2O 240 parts by weight xanthan gum 1 parts by weight

[0199] The slurry was spray-dried to form microsphere particles with a particle size distribution of 20 to 100 m. The particles were calcined in a muffle furnace at 550 C. for 3 hours, yielding a [Zn]HZSM-5 formed molecular sieve with an attrition index of 1.2.

Example 1

[0200] This embodiment employs the device illustrated in the FIGURE.

[0201] Naphtha feedstock fed to the naphtha and methanol coupled aromatization reactor is coal direct liquefaction naphtha with an aromatics potential content of 78 wt %.

[0202] Naphtha and methanol coupled aromatization reaction zone conditions: gas superficial velocity is 0.5 m/s, reaction temperature is 600 C., reaction pressure is 100 kPa, bed density is 700 kg/m.sup.3.

[0203] Regeneration gas is air.

[0204] Regeneration zone conditions in the regenerator: gas superficial velocity is 0.5 m/s, regeneration temperature is 745 C., regeneration pressure is 100 kPa, bed density is 700 kg/m.sup.3.

[0205] Carbon content in the regenerated catalyst is 0.2 wt %.

[0206] Riser reactor feedstock is light alkanes separated from the product gas flow.

[0207] Riser reactor conditions: gas superficial velocity is 3.0 m/s, temperature is 690 C., pressure is 100 kPa, bed density is 150 kg/m.sup.3.

[0208] Bed reactor feedstock is unconverted naphtha separated from the product gas flow, with the main components of the unconverted naphtha being linear aliphatic hydrocarbons, branched aliphatic hydrocarbons and naphthenes of C.sub.4-C.sub.12.

[0209] Light hydrocarbon aromatization reaction zone conditions: gas superficial velocity is 0.5 m/s, reaction temperature is 665 C., reaction pressure is 100 kPa, bed density is 700 kg/m.sup.3.

[0210] Single-pass conversion of naphtha feedstock into the naphtha and methanol coupled aromatization reactor is 60 wt %.

[0211] Product distribution: 72 wt % BTX, 8 wt % light olefins, 3 wt % hydrogen, 3.5 wt % light alkanes, 5 wt % combustible gas, 7.5 wt % heavy aromatics, 1 wt % coke. The content of p-xylene in the mixed xylene in the product is 60 wt %.

Example 2

[0212] This embodiment employs the device illustrated in the FIGURE.

[0213] Naphtha feedstock fed to the naphtha and methanol coupled aromatization reactor is coal direct liquefaction naphtha with an aromatics potential content of 0.1 wt %, including unconverted naphtha recycled from the separated product gas flow.

[0214] Naphtha and methanol coupled aromatization reaction zone conditions: gas superficial velocity is 2.0 m/s, reaction temperature is 510 C., reaction pressure is 500 kPa, bed density is 150 kg/m.sup.3.

[0215] Regeneration gas is oxygen.

[0216] Regeneration zone conditions in the regenerator: gas superficial velocity is 2.0 m/s, regeneration temperature is 610 C., regeneration pressure is 500 kPa, bed density is 150 kg/m.sup.3.

[0217] Carbon content in the regenerated catalyst is 0.1 wt %.

[0218] Riser reactor feedstock is light alkanes separated from the product gas flow and water vapor, with a water vapor content of 80 wt %.

[0219] Riser reactor conditions: gas superficial velocity is 10.0 m/s, temperature is 580 C., pressure is 500 kPa, bed density is 50 kg/m.sup.3.

[0220] Bed reactor feedstock is C.sub.3, C.sub.4, and C.sub.5 hydrocarbons separated from the product gas flow.

[0221] Light hydrocarbon aromatization reaction zone conditions: gas superficial velocity is 2.0 m/s, reaction temperature is 550 C., reaction pressure is 500 kPa, bed density is 150 kg/m.sup.3.

[0222] Single-pass conversion of naphtha feedstock into the naphtha and methanol coupled aromatization reactor is 76 wt %.

[0223] Product distribution: 64 wt % BTX, 14 wt % light olefins, 5.3 wt % hydrogen, 3 wt % light alkanes, 5 wt % combustible gas, 8 wt % heavy aromatics, 0.7 wt % coke. The content of p-xylene in the mixed xylene in the product is 73 wt %.

Example 3

[0224] This embodiment employs the device illustrated in the FIGURE.

[0225] Naphtha feedstock fed to the naphtha and methanol coupled aromatization reactor is coal direct liquefaction naphtha with an aromatics potential content of 3 wt %, including unconverted naphtha recycled from the separated product gas flow.

[0226] Naphtha and methanol coupled aromatization reaction zone conditions: gas superficial velocity is 1.2 m/s, reaction temperature is 550 C., reaction pressure is 120 kPa, bed density is 260 kg/m.sup.3.

[0227] Regeneration gas is oxygen-enriched air.

[0228] Regeneration zone conditions in the regenerator: gas superficial velocity is 1.2 m/s, regeneration temperature is 650 C., regeneration pressure is 120 kPa, bed density is 260 kg/m.sup.3.

[0229] Carbon content in the regenerated catalyst is 0.3 wt %.

[0230] Riser reactor feedstock is light alkanes separated from the product gas flow and water vapor, with a water vapor content of 25 wt %.

[0231] Riser reactor conditions: gas superficial velocity is 7.0 m/s, temperature is 630 C., pressure is 120 kPa, bed density is 80 kg/m.sup.3.

[0232] Bed reactor feedstock is C.sub.4 and C.sub.5 hydrocarbons separated from the product gas flow.

[0233] Light hydrocarbon aromatization reaction zone conditions: gas superficial velocity is 1.2 m/s, reaction temperature is 580 C., reaction pressure is 120 kPa, bed density is 260 kg/m.sup.3.

[0234] Single-pass conversion of naphtha feedstock into the naphtha and methanol coupled aromatization reactor is 80 wt %.

[0235] Product distribution: 60 wt % BTX, 15 wt % light olefins, 7 wt % hydrogen, 7 wt % light alkanes, 5 wt % combustible gas, 5.5 wt % heavy aromatics, 0.5 wt % coke. The content of p-xylene in the mixed xylene in the product is 75 wt %.

Example 4

[0236] This embodiment employs the device illustrated in the FIGURE.

[0237] Naphtha feedstock fed to the naphtha and methanol coupled aromatization reactor is coal direct liquefaction naphtha with an aromatics potential content of 46 wt %, including unconverted naphtha recycled from the separated product gas flow.

[0238] Naphtha and methanol coupled aromatization reaction zone conditions: gas superficial velocity is 1.8 m/s, reaction temperature is 590 C., reaction pressure is 200 kPa, bed density is 220 kg/m.sup.3.

[0239] Regeneration gas is air.

[0240] Regeneration zone conditions in the regenerator: gas superficial velocity is 1.8 m/s, regeneration temperature is 700 C., regeneration pressure is 200 kPa, bed density is 220 kg/m.sup.3.

[0241] Carbon content in the regenerated catalyst is 0.1 wt %.

[0242] Riser reactor feedstock is light alkanes separated from the product gas flow and water vapor, with a water vapor content of 50 wt %.

[0243] Riser reactor conditions: gas superficial velocity is 5.0 m/s, temperature is 660 C., pressure is 220 kPa, bed density is 110 kg/m.sup.3.

[0244] Bed reactor feedstock is C.sub.4 and C.sub.5 hydrocarbons separated from the product gas flow.

[0245] Light hydrocarbon aromatization reaction zone conditions: gas superficial velocity is 1.8 m/s, reaction temperature is 630 C., reaction pressure is 200 kPa, bed density is 220 kg/m.sup.3.