Diethyl oxalate catalysts

Patent metadata

Field	Value
Publication number	US-10549265-B2
Application number	US-201514749222-A
Country	US
Kind code	B2
Filing date	Jun 24, 2015
Priority date	Jun 27, 2014
Publication date	Feb 4, 2020
Grant date	Feb 4, 2020

Abstract

A highly effective catalyst for the preparation of diethyl oxalate using carbon monoxide using Pd/α-Al 2 O 3 and CeO 2 as a promoter. High conversion rates with greatly extended catalyst life is achieved with the CeO 2 -enhanced Pd catalysts. The catalysts can be used for the production of high-value diethyl oxalate, and eventually ethylene glycol, from coal-derived syngas.

First claim

We claim:

1. A highly effective catalyst for the preparation of diethyl oxalate using carbon monoxide, comprising:
an active component;
a carrier; and
a promoter agent,

wherein:
the active component is palladium present in the form of particles and the particles have an average surface area within the range of 2 m 2 /g and 12 m 2 /g;
the carrier is α-alumina:
the promoter agent is CeO 2 the loading of CeO 2 within 0.15 and 0.25 percent by weight; and
the catalyst demonstrates a conversion rate of at least about 62 percent.

2. The catalyst of claim 1 , wherein the loading of active component is within the range of 0.1 and 1 percent by weight.

3. The catalyst of claim 2 , wherein the loading of CeO 2 is 0.2 percent by weight.

4. The catalyst of claim 1 , wherein the active component particles have an average size within the range of 2 and 80 nm and an average surface area within the range of 3 m 2 /g and 8 m 2 /g.

5. The catalyst of claim 1 wherein the carbon monoxide is from coal-derived syngas.

6. A method of improving the conversion rate of carbon monoxide to diethyl oxalate by at least fifty percent by catalysts comprising:
an active component;
a carrier; and
a promoter agent,

wherein:
the active component is palladium present in the form of particles with an average surface area within the range of 3 m 2 /g and 8 m 2 /g;
the carrier is α-alumina; and
the promoter agent is CeO 2 , the loading of CeO 2 within 0.07 and 0.6 percent by weight.

7. The method of claim 6 , wherein the active component is present at about 0.8 to 0.9 percent by weight.

8. The method of claim 7 , wherein the active component particles have a size of between about 9 and 17 nm.

9. The method of claim 8 , wherein the carbon monoxide is from coal derived syngas.

10. The method of claim 4 , wherein the active component particles have a size of between about 9 and 17 nm.

11. The method of claim 10 , wherein the active component is present between about 0.7 and 1 percent by weight.

12. The method of claim 11 , wherein the active component is present at about 0.8 percent by weight and the promoter is present at about 0.2 percent by weight.

13. A method for producing diethyl oxalate comprising:
providing carbon monoxide;
providing ethyl nitrite;
providing a catalyst, the catalyst comprising:
a palladium active agent, wherein:
the palladium is present in the form of particles;
the particles have an average surface area between 2 m 2 /g; and 12 m 2 /g and
the palladium loading is between 0.8 and 0.9% wt.;

a CeO 2 promoter, the CeO 2 loading being between 0.15 and 0.25% wt.; and
an α-alumina carrier; and

reacting the carbon monoxide and ethyl nitrite in the presence of the catalyst,
wherein the reaction has a carbon monoxide conversion rate greater than about 62% and an ethyl nitrite conversion rate of about 92%.

Assignees

• Univ Wyoming

Inventors

• Fan Maohong
• Jin Erlei

Classifications

• C07C67/36

  by reaction with carbon monoxide or formates (C07C67/02, C07C67/03, C07C67/10 take precedence) · CPC title

• B01J23/63 Primary

  with rare earths or actinides · CPC title

• B01J35/1014

  Operations & Transport · mapped topic

• B01J35/1009

  Operations & Transport · mapped topic

• B01J35/023

  Operations & Transport · mapped topic