Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO2 Methanation

Chen, Shenghua1; Zhang, Zedong1; Jiang, Wenjun2; Zhang, Shishi3; Zhu, Jiexin4; Wang, Liqiang5; Ou, Honghui1; Zaman, Shahid6; Tan, Lin6; Zhu, Peng1; Zhang, Erhuan1; Jiang, Peng1; Su, Yaqiong3; Wang, Dingsheng1; Li, Yadong1

2022-07-01

10.1021/jacs.2c03875

Journal of the American Chemical Society   Impact Factor & Quartile

0002-7863

1520-5126

ABSTRACT: The renewable energy-powered electrolytic reduction of carbon dioxide (CO2) to methane (CH4) using water as a reaction medium is one of the most promising paths to store intermittent renewable energy and address global energy and sustainability problems. However, the role of water in the electrolyte is often overlooked. In particular, the slow water dissociation kinetics limits the proton-feeding rate, which severely damages the selectivity and activity of the methanation process involving multiple electrons and protons transfer. Here, we present a novel tandem catalyst comprising Ir single-atom (Ir1)-doped hybrid Cu3N/Cu2O multisite that operates efficiently in converting CO2 to CH4. Experimental and theoretical calculation results reveal that the Ir1 facilitates water dissociation into proton and feeds to the hybrid Cu3N/Cu2O sites for the *CO protonation pathway toward *CHO. The catalyst displays a high Faradaic efficiency of 75% for CH4 with a current density of 320 mA cm-2 in the flow cell. This work provides a promising strategy for the rational design of high-efficiency multisite catalytic systems.

SCI ; EI

English

NI Journal Papers ; NI论文

Others

National Key R&D Program of China["2020YFA0710304","2018YFA0702003"] ; National Natural Science Foundation of China["22002185","21890383","21871159","22171157"] ; Science and Technology Key Project of Guangdong Province of China[2020B010188002] ; China Postdoctoral Science Foundation[2021M691749]

Chemistry

Chemistry, Multidisciplinary

WOS:000826699200001

AMER CHEMICAL SOC

20223312580004

Dissociation ; Electrocatalysts ; Electrolytes ; Electrolytic reduction ; Molecules

Ore Treatment:533.1 ; Electric Batteries and Fuel Cells:702 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

Web of Science

1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.China Acad Space Technol, Qian Xuesen Lab Space Technol, Beijing 100094, Peoples R China
3.Xi An Jiao Tong Univ, Sch Chem, Xian Key Lab Sustainable Energy Mat Chem, State Key Lab Elect Insulat & Power Equipment, Xian 710049, Peoples R China
4.Wuhan Univ Technol, State Key Lab Adv Technol Mat Synthesis & Proc, Int Sch Mat Sci & Engn, Wuhan 430070, Peoples R China
5.Zhengzhou Univ, Henan Prov Ind Technol Res Inst Resources & Mat, Sch Mat Sci & Engn, Zhengzhou 450001, Peoples R China
6.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Key Lab Energy Convers & Storage Technol, Shenzhen 518055, Peoples R China

Chen, Shenghua,Zhang, Zedong,Jiang, Wenjun,et al. Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO2 Methanation[J]. Journal of the American Chemical Society,2022,144:12807-12815.

Chen, Shenghua.,Zhang, Zedong.,Jiang, Wenjun.,Zhang, Shishi.,Zhu, Jiexin.,...&Li, Yadong.(2022).Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO2 Methanation.Journal of the American Chemical Society,144,12807-12815.

Chen, Shenghua,et al."Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO2 Methanation".Journal of the American Chemical Society 144(2022):12807-12815.