# US 8,772,564 B2 · Method of producing synthetic zeolite catalyst and method of producing high-purity paraxylene with a catalyst produced by such a method

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- Number: US 8,772,564 B2
- Document ID: US8772564B2
- Status: Granted
- Kind: B2
- Application number: 13/119,825
- Filed: 2009-09-29
- Published: 2011-08-18
- Granted: 2014-07-08
- Earliest claimed: 2008-10-09
- Assignees: Jx Nippon Oil & Energy Corporation
- Applicants: Koichi Matsushita; Chikanori Nakaoka; Norikazu Nishiyama
- Inventors: Koichi Matsushita; Chikanori Nakaoka; Norikazu Nishiyama
- Web page: https://patentgrep.com/patent/US8772564B2

## CPC

- C07C 2/865: {the non-hydrocarbon is an ether}
- B01J 29/005: {Mixtures of molecular sieves comprising at least one molecular sieve which is not an aluminosilicate zeolite, e.g. from groups B01J29/03 - B01J29/049 or B01J29/82 - B01J29/89}
- B01J 29/80: Mixtures of different zeolites
- B01J 35/40: characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77)
- C01B 39/40: using at least one organic template directing agent
- C01B 39/48: using at least one organic template directing agent
- C01B 39/54: Phosphates, e.g. APO or SAPO compounds
- C07C 2/864: {the non-hydrocarbon is an alcohol}
- C07C 6/123: {of only one hydrocarbon}
- B01J 29/035: {Microporous crystalline materials not having base exchange properties, such as} silica polymorphs, e.g. silicalites
- B01J 29/40: of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively
- B01J 29/85: Silicoaluminophosphates [SAPO compounds]
- B01J 2229/12: to alter the outside of the crystallites, e.g. selectivation
- B01J 2229/32: Reaction with silicon compounds, e.g. TEOS, siliconfluoride
- B01J 2229/62: in or on other molecular sieves
- C07C 2529/70: of types characterised by their specific structure not provided for in groups C07C2529/08 - C07C2529/65
- Y02P 20/52: using catalysts, e.g. selective catalysts
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

This invention relates to a method wherein a high-purity paraxylene can be produced efficiently by using a catalyst having a molecular sieving action (or shape selectivity) and being excellent in the catalytic activity without isomerization and adsorption-separation steps. More particularly, it relates to a method of producing a high-purity paraxylene, characterized in that MFI type zeolite having a primary particle size of not more than 100 μm, a structure defining agent and silica material having an average particle size of not less than 10 nm but less than 1.0 μm are used as a starting material, and a synthetic zeolite catalyst produced by subjecting the MFI type zeolite to a coating treatment with an aqueous solution obtained by mixing so as to satisfy X×Y<0.05 (wherein X is a concentration of the silica material (mol %) and Y is a concentration of the structure defining agent (mol %)) is used in the alkylation or disproportionation of at least one of benzene and toluene as a starting material.

## Claims

### Claim 1

A method of producing a synthetic zeolite catalyst by coating MFI type zeolite having a primary particle size of not more than 100 μm with a monocrystalline silicate, wherein the MFI type zeolite is subjected to a coating treatment in which the MFI type zeolite is immersed into an aqueous solution obtained by mixing a structure defining agent and a silica material having an average particle size of not less than 10 nm but less than 1.0 μm so as to satisfy X×Y<0.05 (wherein X is a concentration of the silica material (mol %) and Y is a concentration of the structure defining agent (mol %)), then subjected to a hydrothermal treatment at a temperature of 120° C. to 250° C. for 0.5 hour to 48 hours and further fired.

### Claim 2 (depends on 1)

The method of producing a synthetic zeolite catalyst according to claim 1, wherein the monocrystalline silicate is silicalite.

### Claim 3 (depends on 1)

A method of producing a high-purity paraxylene, which comprises the step of subjecting at least one of benzene and toluene as a starting material to an alkylation or a disproportionation in the presence of a synthetic zeolite catalyst produced by a method as claimed in claim 1 at a liquid hourly space velocity of 0.01 h−1 to 10 h−1 and a temperature of 200° C. to 550° C.

### Claim 4 (depends on 3)

The method of producing a high-purity paraxylene according to claim 3, wherein a conversion of toluene is not less than 30 mol %, and a selectivity of paraxylene in aromatic hydrocarbons having a carbon number of 8 is not less than 97.5 mol %.

### Claim 5 (depends on 2)

A method of producing a high-purity paraxylene, which comprises the step of subjecting at least one of benzene and toluene as a starting material to an alkylation or a disproportionation in the presence of a synthetic zeolite catalyst produced by a method as claimed in claim 2 at a liquid hourly space velocity of 0.01 h−1 to 10 h−1 and a temperature of 200° C. to 550° C.