Method for preparing acetal carbonyl compound

Patent metadata

Field	Value
Publication number	US-10508073-B2
Application number	US-201515743698-A
Country	US
Kind code	B2
Filing date	Dec 8, 2015
Priority date	Jul 20, 2015
Publication date	Dec 17, 2019
Grant date	Dec 17, 2019

Abstract

The present application provides a method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol, which comprises a step in which a raw material acetal and a raw gas carbon monoxide go through a reactor loaded with a catalyst containing an acidic microporous silicoaluminophosphate molecular sieve, for carrying out a carbonylation reaction. In the method of the present invention, the conversion rate of the raw material acetal is high, and the selectivity of acetal carbonylation is high, and the catalyst life is long, and no additional solvent is needed in the reaction process, and the reaction condition is relatively mild, and the process is continuous, showing the potential for industrial application. Moreover, the product of acetal carbonyl compound can be used for producing ethylene glycol by hydrogenation followed by hydrolysis.

First claim

The invention claimed is:

1. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol, which comprises a step in which a raw material acetal and carbon monoxide go through a reactor loaded with a catalyst for carrying out a carbonylation reaction; wherein the catalyst contains an acidic microporous silicoaluminophosphate molecular sieve; wherein the chemical composition of the acidic microporous silicoaluminophosphate molecular sieve is expressed as (Si x Al y P z )O 2 , and x is in a range from 0.01 to 0.60, and y is in a range from 0.2 to 0.60, and z is in a range from 0.2 to 0.60, and x+y+z=1; wherein the raw material acetal is expressed as R 1 O(CH 2 O) n R 2 , and n is selected from 1, 2, 3 or 4, and R 1 and R 2 are independently selected from C 1 -C 3 alkyls; wherein the acidic microporous silicoaluminophosphate molecular sieve is one or more molecular sieves selected from the molecular sieves with framework type of CHA, RHO, LEV, ERI, AEI or AFX.

2. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the acidic microporous silicoaluminophosphate molecular sieve ahas an 8-membered ring pore framework.

3. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the acidic microporous silicoaluminophosphate molecular sieve is one or more molecular sieves selected from SAPO-34, DNL-6, SAPO-35, SAPO-17, SAPO-18 or SAPO-56.

4. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the acidic microporous silicoaluminophosphate molecular sieve contains a metal; and the mass fraction of the metal element in the acidic microporous silicoaluminophosphate molecular sieve is in a range from 0% to 10%.

5. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 4 , wherein the metal is located at the ion-exchange sites, in the pores and channels, on the surface and/or in the framework of the acidic microporous silicoaluminophosphate molecular sieve; and the metal is introduced by one or more methods selected from in-situ synthesis, impregnation or ion exchange.

6. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the catalyst contains a forming agent, and the mass fraction of the forming agent in the catalyst is in a range from 10% to 60%.

7. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the raw material acetal is CH 3 OCH 2 OCH 3 , C 2 H 5 OCH 2 OC 2 H 5 or CH 3 O(CH 2 O) 2 CH 3 , and the acetal carbonyl compound is one or more compounds selected from CH 3 —O—(CO)—CH 2 —O—CH 3 , C 2 H 5 —O—(CO)—CH 2 —O—C 2 H 5 , CH 3 —O—(CO)—CH 2 —O—CH 2 —O—CH 3 or CH 3 —O—CH 2 —(CO)—O—CH 2 —O—CH 3 .

8. A method for preparing acetal carbonyl compound used as n intermediate for producing ethylene glycol according to claim 1 , wherein the carbonylation reaction conditions are as follows: the reaction temperature is in a range from 60° C. to 140° C., and the reaction pressure is in a range from 1 MPa to 15 MPa, and the mass space velocity of the raw material acetal is in a range from 0.1 h −1 to 10.0 h −1 , and the molar ratio of carbon monoxide to the raw material acetal is in a range from 2:1 to 20:1, and no solvent is added.

9. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the reactor is a continuous reactor which is selected from a fixed bed reactor, a tank reactor, a moving bed reactor or a fluidized bed reactor.

10. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 4 , wherein the mass fraction of the metal element in the acidic microporous silicoaluminophosphate molecular sieve is in a range from 0% to 2%.

11. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 4 , wherein the metal is one or more metals selected from copper, iron, gallium, silver, nickel, cobalt, palladium or platinum.

12. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 6 , wherein the mass fraction of the forming agent in the catalyst is in a range from 10% to 30%.

13. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 6 , wherein the forming agent is one or more compounds selected from alumina, silicon oxide or kaolin.

14. A method for preparing acetal carbonyl compound used as an intermediate for producing ethylene glycol according to claim 1 , wherein the carbonylation reaction conditions are as follows: the reaction temperature is in a range from 70° C. to 120° C., and the reaction pressure is in a range from 3 MPa to 10 MPa, and the mass space velocity of the raw material acetal is in a range from 0.5 h −1 to 3 h −1 , and the molar ratio of carbon monoxide to the raw material acetal is in a range from 5:1 to 15:1, and no solvent is added.

Assignees

• Dalian Inst Chem & Physics Cas

Inventors

• Ni Youming
• Zhu Wenliang
• Liu Yong
• Liu Hongchao
• Liu Zhongmin
• Yang Miao
• Tian Peng

Classifications

• B01J2523/17

  Copper · CPC title

• C01B37/08

  Silicoaluminophosphates [SAPO compounds] {, e.g. CoSAPO} · CPC title

• C07C67/37 Primary

  by reaction of ethers with carbon monoxide · CPC title

• B01J2229/183

  in framework positions · CPC title

• C07C69/708

  Ethers · CPC title