Methods, systems and catalysts for oxidizing carbon monoxide to carbon dioxide

Patent metadata

Field	Value
Publication number	US-10130941-B2
Application number	US-201415117426-A
Country	US
Kind code	B2
Filing date	Feb 7, 2014
Priority date	Feb 7, 2014
Publication date	Nov 20, 2018
Grant date	Nov 20, 2018

Abstract

Methods and catalyst compositions for oxidizing CO to CO 2 at low temperatures are disclosed. In one embodiment, a method of oxidizing CO to CO 2 may involve heating a gaseous mixture comprising at least CO and O 2 with a catalyst mixture comprising Pd disposed on a Mn 3 O 4 mesoporous support at a temperature of about 0° C. to about 60° C., and wherein the CO to CO 2 conversion rate is about 40% to about 100%.

First claim

What is claimed is:

1. A method to oxidize CO to CO 2 , the method comprising:
forming a mesoporous Mn 3 O 4 support, wherein the forming comprises:
mixing a triblock copolymer, a manganese salt, and a solvent to form a solution,

wherein the triblock copolymer is poly(ethyleneglycol)-poly(propyleneglycol)-poly(ethyleneglycol), poly(ethyleneimine)-poly(ethyleneglycol)-poly(ethyleneimine), poly(ethyleneglycol)-polyacetal-poly(ethyleneglycol), polyacetal-poly(ethyleneglycol)-polyacetal, or any combinations thereof;
evaporating the solution; and
calcining to form the mesoporous Mn 3 O 4 support;

contacting the mesoporous Mn 3 O 4 support with a Pd compound to form a reaction mixture;
contacting the reaction mixture with a reducing agent to form a catalyst mixture; isolating the catalyst mixture; and
contacting a gaseous mixture and the catalyst mixture at a temperature of about 0° C. to about 60° C., wherein the gaseous mixture comprises CO and O 2 , and
wherein the CO is converted to CO 2 at a conversion rate of about 40% to about 100%.

2. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting with the catalyst mixture that comprises at least one Pd nanoparticle disposed on at least a portion of the mesoporous Mn 3 O 4 support.

3. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting at a temperature of about 20° C. to about 30° C., and wherein the CO is converted to CO 2 at a conversion rate of about 80% to about 100%.

4. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting at a temperature of about 0° C. to about 10° C., and wherein the CO is converted to CO 2 at a conversion rate of about 40% to about 50%.

5. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting the gaseous mixture that further comprises N 2 , He, H 2 , Ar, or any combination thereof.

6. The method of claim 1 , wherein the method comprises a batch process or a continuous flow process.

7. The method of claim 6 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting in the continuous flow process, where the gaseous mixture is in contact with the catalyst mixture at a flow rate of about 40 mL per minute to about 60 mL per minute.

8. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting with the catalyst mixture that includes about 1 weight percent to about 5 weight percent of Pd.

9. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting with the catalyst mixture that includes the mesoporous Mn 3 O 4 support having an average pore diameter of about 1 nanometer to about 50 nanometer.

10. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting the gaseous mixture that further comprises water.

11. The method of claim 1 , wherein contacting the gaseous mixture and the catalyst mixture comprises contacting the gaseous mixture that includes about 1 volume percent to about 10 volume percent CO.

12. A method to make a Pd/Mn 3 O 4 catalyst, the method comprising:
forming Mn 3 O 4 support, wherein the forming comprises:
mixing a triblock copolymer, a manganese salt, and a solvent to form a solution, wherein the triblock copolymer is poly(ethyleneglycol)-poly(propyleneglycol)-poly(ethyleneglycol), poly(ethyleneimine)-poly(ethyleneglycol)-poly(ethyleneimine), poly(ethyleneglycol)-polyacetal-poly(ethyleneglycol), polyacetal-poly(ethyleneglycol)-polyacetal, or any combinations thereof;
evaporating the solution; and
calcining to form the Mn 3 O 4 support,

contacting the Mn 3 O 4 support with a Pd compound to form a reaction mixture, contacting the reaction mixture with a reducing agent to form a precipitate, and isolating the precipitate.

13. The method of claim 12 , wherein contacting the Mn 3 O 4 support with the Pd compound comprises contacting a mesoporous Mn 3 O 4 support.

14. The method of claim 12 , wherein mixing the triblock copolymer, the manganese salt, and the solvent comprises mixing the manganese salt selected from the group consisting of Mn(NO 3 ) 2 , MnCl 2 , MnBr 2 , MnF 2 , MnPO 4 , MnSO 4 , or any combination thereof.

15. The method of claim 12 , wherein evaporating the solution comprises heating the solution to a temperature of about 50° C. to about 80° C. for about 24 hours to about 96 hours.

16. The method of claim 12 , wherein calcining the Mn 3 O 4 support comprises heating the Mn 3 O 4 support to a temperature of about 300° C. to about 600° C. for about 30 minutes to about 6 hours.

17. The method of claim 12 , wherein contacting the Mn 3 O 4 support with the Pd compound comprises contacting with Na 2 PdCl 4 , H 2 PdCl 4 , K 2 PdCl 4 , (NH 4 ) 2 PdCl 4 , Pd(CH 3 COO) 2 , Pd(NO 3 ) 2 , PdSO 4 , or any combination thereof.

18. The method of claim 12 , wherein contacting with the reducing agent comprises contacting with hydrazine, NaBH 4 , KBH 4 , or any combination thereof.

19. The method of claim 12 , wherein isolating the precipitate comprises removing the precipitate from the reaction mixture by centrifugation, filtration, distillation, decantation, or any combination thereof.

Assignees

• Univ East China Science & Tech

Inventors

• Li Liang
• Li Gengnan

Classifications

• B01D2255/9207

  Specific surface · CPC title

• B01J37/16

  Reducing · CPC title

• B01J35/1057

  Operations & Transport · mapped topic

• B01J37/031

  Precipitation · CPC title

• B01J37/035

  Precipitation on carriers · CPC title