Carbon supported single atom carbon dioxide reduction electro catalysts

Patent metadata

Field	Value
Publication number	US-2019276943-A1
Application number	US-201815915259-A
Country	US
Kind code	A1
Filing date	Mar 8, 2018
Priority date	Mar 8, 2018
Publication date	Sep 12, 2019
Grant date	—

Abstract

Electrocatalysts composed of single atoms dispersed over porous carbon support were prepared by a lithium-melt method. The new catalysts demonstrated high selectivity, high Faradic efficiency and low overpotential toward to the electrocatalytic reduction of carbon dioxide to fuels.

First claim

1 . A method of synthesizing a catalyst comprising:
adding a catalytic metal in its metallic form to molten alkaline metal; atomically dispersing the catalytic metal in the molten alkaline metal; forming an alkaline metal-catalytic metal solid; converting a portion of alkaline metal in the alkaline metal-catalytic metal solid to alkaline metal hydroxide forming a metal-alkaline metal hydroxide solid; mixing said metal-alkaline metal hydroxide solid with a conductive support material to form a mixture; removing alkaline metal hydroxide from the mixture leaving a mixture of metal in the conductive support; and drying the mixture of metal and the conductive support to produce the catalyst containing the catalytic metal atomically dispersed over the conductive support.

2 . The method of claim 1 , wherein the molten alkaline metal is lithium.

3 . The method of claim 2 , wherein converting the portion of the lithium-catalytic metal to metal-lithium hydroxide solid comprises reacting lithium in the metal-lithium solid with the moist air.

4 . The method of claim 2 , further comprising mixing the metal-lithium hydroxide solid with a conductive support material using mechanical method such as ball milling.

5 . The method of claim 2 , wherein the catalytic metal before adding to molten lithium is in metallic state and in the form of power, ingot, wire and shredded pieces.

6 . The method of claim 2 , wherein the catalytic metal is a transition metal.

7 . The method of claim 2 , wherein the catalytic metal is a platinum group metal.

8 . The method of claim 2 , wherein the catalytic metal is dispersed in a single atom form.

9 . The method of claim 1 , wherein the conductive support material is a carbonaceous material.

10 . The method of claim 9 , wherein the carbonaceous material is a porous network and further catalytic metal is decorated through the porous network of carbonaceous material.

11 . The method of claim 9 , wherein removing the metal hydroxide comprises washing the metal-lithium hydroxide with water thereby removing lithium.

12 . The method of claim 10 , wherein the washing comprises forming an alkaline water solution and modifying the carbonaceous support with the oxygenated species serving as anchoring sites for the catalytic metal.

13 . The catalytic material of claim 11 having a catalytic selectivity of at least 95% and Faradaic efficiency of at least 93% in converting of carbon dioxide to ethanol

14 . The catalytic material of claim 11 having a catalytic selectivity of about 100% and Faradaic efficiency of higher than 97% in converting carbon dioxide to acetone.

15 . The catalytic material of claim 1 , wherein the catalytic metal is a bimetallic compound.

16 . A method of synthesizing a catalyst comprising:
forming an dispersion of multiple metals in a molten alkaline metal; forming an alkaline metal-multiple metal solid; converting a portion of alkaline metal in the alkaline metal-first catalytic metal-second catalytic metal solid to an alkaline metal hydroxide forming an alkaline metal hydroxide-multiple metal solid; mixing said alkaline metal hydroxide-multiple metal solid with a conductive support material; removing alkaline metal hydroxide from the mixture of the alkaline metal hydroxide-multiple metal solid and a conductive support; and drying the multiple metal and conductive support mixture to produce the catalyst containing the multiple metals atomically dispersed over the conductive support.

17 . The method of claim 16 , wherein forming the dispersion of multiple metals comprises:
adding a first catalytic metal in its metallic form to the molten alkaline metal; and adding a second catalytic metal in its metallic form to the molten alkaline metal;

18 . The method of claim 16 , wherein forming the dispersion of multiple metals comprises adding a multi-metallic catalytic compound to the molten alkaline metal.

19 . The method of claim 16 , wherein the conductive support material is a carbonaceous material having porous network and further catalytic metal is decorated through the porous network of carbonaceous material.

20 . The method of claim 16 , wherein removing the metal hydroxide comprises forming an alkaline water solution and modifying the carbonaceous support with the oxygenated species serving as anchoring sites for the catalytic metal.

Assignees

• Uchicago Argonne Llc

Inventors

• Liu Di-Jia
• Xu Tao
• Rebollar Dominic
• Xu Haiping

Classifications

• B01J19/087

  employing electric or magnetic energy · CPC title

• C07C45/00

  Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds · CPC title

• C07C29/154

  containing copper, silver, gold, or compounds thereof · CPC title

• B01J2219/0875

  Gas · CPC title

• B01J2219/0803

  employing electric or magnetic energy · CPC title