Methyl acetate preparation method

Patent metadata

Field	Value
Publication number	US-10287233-B2
Application number	US-201515743936-A
Country	US
Kind code	B2
Filing date	Dec 8, 2015
Priority date	Jul 20, 2015
Publication date	May 14, 2019
Grant date	May 14, 2019

Abstract

The present invention provides a method for producing methyl acetate, and the method comprises a step in which dimethyl ether and a raw gas containing carbon monoxide and hydrogen go through a reactor loaded with a catalyst for carrying out a carbonylation reaction; wherein the catalyst contains an acidic EMT zeolite molecular sieve. The present invention has provided a new method for producing methyl acetate. In the method of the present invention, the carbonylation is carried out in the presence of the catalyst containing the acidic EMT zeolite molecular sieve, and the reaction activity is high, and the stability has been significantly improved, meeting the requirement of industrial production.

First claim

The invention claimed is:

1. A method for producing methyl acetate, which comprises a step in which dimethyl ether and a raw gas containing carbon monoxide go through a reactor loaded with a catalyst for carrying out a carbonylation reaction; wherein the catalyst contains an acidic EMT zeolite molecular sieve.

2. A method for producing methyl acetate according to claim 1 , wherein in the acidic EMT zeolite molecular sieve, the molar ratio of silicon atoms to aluminum atoms is in a range from 1.5 to 30.

3. A method for producing methyl acetate according to claim 1 , wherein the acidic EMT zeolite molecular sieve contains a catalyst promoter which is one or more metals selected from gallium, iron, copper and silver.

4. A method for producing methyl acetate according to any of claims 1 to 3 , wherein the acidic EMT zeolite molecular sieve contains a binder which is one or more compounds selected from alumina, silicon dioxide and magnesium oxide.

5. A method for producing methyl acetate according to claim 1 , wherein the carbonylation reaction is carried out at a temperature range from 160° C. to 250° C. and at a pressure range from 0.5 MPa to 20.0 MPa, and the feeding mass space velocity of dimethyl ether is in a range from 0.05 −1 to 3 h −1 , and the molar ratio of carbon monoxide to dimethyl ether is in a range from 20:1 to 0.5:1.

6. A method for producing methyl acetate according to claim 1 , wherein the carbonylation reaction is carried out at a temperature range from 170° C. to 240° C. and at a pressure range from 1.0 MPa to 15.0 MPa, and the feeding mass space velocity of dimethyl ether is in a range from 0.1h −1 to 2.5h −1 , and the molar ratio of carbon monoxide to dimethyl ether is in a range from 15:1 to 1:1.

7. A method for producing methyl acetate according to claim 1 , wherein the raw gas containing carbon monoxide contains carbon monoxide, hydrogen and one or more inactive gases selected from nitrogen, helium, argon, carbon dioxide, methane and ethane.

8. A method for producing methyl acetate according to claim 1 , wherein the methyl acetate is hydrolyzed to acetic acid.

9. A method for producing methyl acetate according to claim 1 , wherein the methyl acetate is hydrogenated to ethyl alcohol.

10. A method for producing methyl acetate according to claim 1 , wherein the carbonylation reaction is carried out in a fixed bed reactor, a fluidized bed reactor or a moving bed reactor.

11. A method for producing methyl acetate according to claim 1 , wherein in the acidic EMT zeolite molecular sieve, the molar ratio of silicon atoms to aluminum atoms is in a range from 2 to 15.

12. A method for producing methyl acetate according to claim 3 , wherein the catalyst promoter is introduced to the acidic EMT zeolite molecular sieve by a method selected from in-situ synthesis, metal ion exchange or impregnation loading.

13. A method for producing methyl acetate according to claim 3 , wherein based on the total weight of the catalyst, the weight fraction of the catalyst promoter calculated by weight of metal elementary substance is in a range from 0.01 wt % to 10 wt %.

14. A method for producing methyl acetate according to claim 3 , wherein based on the total weight of the catalyst, the weight fraction of the catalyst promoter calculated by weight of metal elementary substance is in a range from 0.05 wt % to 1.0 wt %.

15. A method for producing methyl acetate according to any of claims 4 , wherein based on the total weight of the catalyst, the weight fraction of the binder is in a range from 0 wt % to 50 wt %.

16. A method for producing methyl acetate according to claim 7 , wherein based on the total volume of the raw gas containing carbon monoxide, the volume fraction of carbon monoxide is in a range from 50% to 100%, and the volume fraction of hydrogen is in a range from 0% to 50%, and the volume fraction of the in-ert gas is in a range from 0% to 50%.

Assignees

• Dalian Inst Chem & Physics Cas

Inventors

• Liu Hongchao
• Zhu Wenliang
• Liu Yong
• Ni Youming
• Liu Zhongmin
• Wang Linying
• Tian Peng

Classifications

• C07C67/37 Primary

  by reaction of ethers with carbon monoxide · CPC title

• B01J29/7019

  EMT-type, e.g. EMC-2, ECR-30, CSZ-1, ZSM-3 or ZSM-20 · CPC title

• B01J29/7069

  EMT-type, e.g. EMC-2, ECR-30, CSZ-1, ZSM-3 or ZSM-20 · CPC title

• B01J29/7638

  EMT-type, e.g. EMC-2, ECR-30, CSZ-1, ZSM-3 or ZSM-20 · CPC title

• C07C29/147

  of carboxylic acids or derivatives thereof · CPC title