Atomic Cu Sites Engineering Enables Efficient CO_(2)Electroreduction to Methane with High CH_(4)/C_(2)H_(4)Ratio  

作　　者：Minhan Li Fangzhou Zhang Min Kuang Yuanyuan Ma Ting Liao Ziqi Sun Wei Luo Wan Jiang Jianping Yang 

机构地区：[1]Institute of Functional Materials,State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,College of Materials Science and Engineering,Donghua University,Shanghai 201620,People’s Republic of China [2]College of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450001,People’s Republic of China [3]School of Mechanical,Medical and Process Engineering,School of Chemistry and Physics,Queensland University of Technology,2 George Street,Brisbane,QLD 4001,Australia

出　　处：《Nano-Micro Letters》2023年第12期361-375,共15页纳微快报（英文版）

基　　金：This work was supported by the Fundamental Research Funds for the Central Universities(2232021A-02 and 2232023Y-01);the National Natural Science Foundation of China(Nos.52122312,22209024 and 22202183).

摘　　要：Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.

关 键 词：CO_(2)RR Cu single-atom catalyst g-C_(3)N_(4) METHANE CH_(4)/C_(2)H_(4)ratio 

分 类 号：TQ426[化学工程] TQ221.11