Copper-tetracyanoquinodimethane-derived copper electrocatalysts for highly selective carbon dioxide reduction to ethylene  

作　　者：Xuewei Huang Dawei Wang Shuhao Yan Pengfei An Jianyu Han Zhiyu Guo Xinwei Li Zhongjun Chen Lin Chang Siyu Lu Zhiyong Tang 

机构地区：[1]Green Catalysis Center,and College of Chemistry,Zhengzhou University,Zhengzhou 450001,China [2]Henan Institute of Advanced Technology,Zhengzhou University,Zhengzhou 450001,China [3]CAS Key Laboratory of Nanosystem and Hierarchical Fabrication,CAS Center for Excellence in Nanoscience,National Center for Nanoscience and Technology,Beijing 100190,China [4]University of Chinese Academy of Sciences,Beijing 100049,China [5]Institute of High Energy Physics Chinese Academy of Sciences,Beijing 100049,China

出　　处：《Nano Research》2022年第9期7910-7916,共7页纳米研究（英文版）

基　　金：the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000,Z.Y.T.);National Key Basic Research Program of China(No.2021YFA1200302,Z.Y.T.);National Natural Science Foundation of China(Nos.92056204,21890381,and 21721002,Z.Y.T.);of 1W1B and 4B9A beamline of Beijing Synchrotron Radiation Facility(BSRF).

摘　　要：As one of the most promising CO_(2)utilization techniques,electrochemical CO_(2)reduction has recently received considerable attention.Cu is a unique electrocatalyst that can convert CO_(2)to value-added multi-carbon chemicals.Nevertheless,Cu catalysts are always limited by the poor selectivity and stability.Here,we report that using copper-tetracyanoquinodimethane(CuTCNQ)derived Cu nanoparticles as efficient electrocatalysts for conversion of CO_(2)to ethylene characteristic with high selectivity and stability,showing 56%Faradaic efficiency(FE)to C2H4 at−1.3 V vs.reversible hydrogen electrode(RHE).Upon the electrochemical CO_(2)reduction,CuTCNQ slowly reconstructs to Cu nanoparticles with abundant grain boundaries and residual Cu+on the surface.Theoretical calculation and operando characterization disclose that both as-formed Cu nanoparticle grain boundaries and residual Cu+endow the catalyst with high selectivity toward ethylene.Furthermore,during the reconstruction of CuTCNQ to Cu nanoparticles,the grain boundaries Cu surface is slowly refreshed by continual addition of Cu atoms,thus inhibiting the surface passivation and guaranteeing the electrocatalytic stability.

关 键 词：reconstruction grain boundary ETHYLENE CO_(2)electroreduction 

分 类 号：O64[理学—物理化学]