Electronic perturbation of Cu nanowire surfaces with functionalized graphdiyne for enhanced CO2 reduction reaction

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外文摘要：Electronic perturbation of the surfaces of Cu catalysts is crucial for optimizing electrochemical CO2 reduction activity,yet still poses great challenges.Herein,nanostructured Cu nanowires(NW)with fine-tuned surface electronic structure are achieved via surface encapsulation with electron-withdrawing(-F)and-donating(-Me)group-functionalized graphdiynes(R-GDY,R=-F and-Me)and the resulting catalysts,denoted as R-GDY/Cu NW,display distinct CO2 reduction performances.In situ electrochemical spectroscopy revealed that the *CO(a key intermediate of the CO2 reduction reaction)binding affinity and consequent *CO coverage positively correlate with the Cu surface oxidation state,leading to favorable C-C coupling on F-GDY/Cu NW over Me-GDY/Cu NW.Electrochemical measurements corroborate the favorable C2H4 production with an optimum C2+selectivity of 73.15％±2.5％observed for F-GDY/Cu NW,while the predominant CH4 production is favored by Me-GDY/Cu NW.Furthermore,by leveraging the*Cu-hydroxyl(OH)/*CO ratio as a descriptor,mechanistic investigation reveals that the protonation of distinct adsorbed *CO facilitated by*Cu-OH is crucial for the selective generation of C2H4 and CH4 on F-GDY/Cu NW and Me-GDY/Cu NW,respectively.

外文关键词：

CO2 reduction reactioncopper nanowiregroup-functionalized graphdiynesurface electronic perturbation

作者：

Haiyuan Zou、Dongfang Cheng、Chao Tang、Wen Luo、Huatian Xiong、Hongliang Dong、Fan Li、Tao Song、Siyan Shu、Hao Dai、Ziang Cui、Zhouguang Lu、Lele Duan

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作者单位：

Department of Chemistry,Southern University of Science and Technology,Shenzhen 518055,China

Department of Chemical and Biomolecular Engineering,University of California Los Angeles,Los Angeles 90095,USA

Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen 518055,China

Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry,School of Science,Westlake University,Hangzhou 310030,China

Center for High-Pressure Science and Technology Advanced Research,Shanghai 201203,China

Department of Chemistry,Tsinghua University,Beijing 100084,China

Division of Solar Energy Conversion and Catalysis at Westlake University,Zhejiang Baima Lake Laboratory Co.,Ltd,Hangzhou 310000,China

Institute of Natural Sciences,Westlake Institute for Advanced Study,Hangzhou 310024,China

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出版年：

2024

DOI：

10.1093/nsr/nwae253

国家科学评论(英文版)

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ISSN：

年,卷(期)：2024.11(12)