Porous copper cluster-based MOF with strong cuprophilic interactions for highly selective electrocatalytic reduction of CO_(2) to CH4  

作　　者：Long-Zhang Dong Yun-Feng Lu Rui Wang Jie Zhou Yu Zhang Lei Zhang Jiang Liu Shun-Li Li Ya-Qian Lan 

机构地区：[1]National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs,Engineering Research Center of MTEES(Ministry of Education),Key Lab.of ETESPG(GHEI),School of Chemistry,South China Normal University,Guangzhou,510006,China [2]Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials,Jiangsu Key Laboratory of New Power Batteries,School of Chemistry and Materials Science,Nanjing Normal University,Nanjing,210023,China

出　　处：《Nano Research》2022年第12期10185-10193,共9页纳米研究（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(Nos.21871141,21871142,22071109,22105080,and 92061101);the Excellent Youth Foundation of Jiangsu Natural Science Foundation(No.BK20211593);Priority Academic Program Development of Jiangsu Higher Education Institutions,and the Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials.

摘　　要：It is well known that the low-valent Cu species are important catalytically active centers in the reduction of CO_(2) to hydrocarbon products.However,the Cu(l)-based catalysts are easily reduced during the electroreduction of CO_(2),which causes phase transformation of catalysts and leads to a decrease of intrinsic catalytic activity.Therefore,it is of great significance to synthesize Cu(l)-based catalysts with specific interactions that can keep the catalytically active Cu sites stable in the electrocatalytic process.Based on the above considerations,a hexanuclear Cu cluster with strong cuprophilic interactions has been designed and utilized as a secondary building unit(SBU)to construct a stable metal-organic framework(MOF)electrocatalyst(NNU-50).As expected,the NNU-50 has served as an effective electrocatalyst for the CO_(2)-to-CH4 conversion by exhibiting a high Faradaic efficiency for CH4(FEcH4)of 66.40%and a large current density of~400 mA·cm-2 at-1.0 V vs.reversible hydrogen electrode(RHE),which is one of the best catalytic performances among the stable MOF electrocatalysts until now.This work contributes more ideas for the design of stable and efficient MOF-based electrocatalysts for CO_(2) reduction reaction.

关 键 词：metal-organic framework cuprophilic interactions carbon dioxide ELECTROREDUCTION 

分 类 号：O64[理学—物理化学]