Boosting electrocatalytic selectivity in carbon dioxide reduction:The fundamental role of dispersing gold nanoparticles on silicon nanowires  

作　　者：Fan Liao Xing Fan Huixian Shi Qing Li Mengjie Ma Wenxiang Zhu Haiping Lin Youyong Li Mingwang Shao 

机构地区：[1]Institute of Functional Nano&Soft Materials(FUNSOM),Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices,Soochow University,Suzhou 215123,China [2]School of Physics and Information Technology,Shaanxi Normal University,Xi'an 710062,China

出　　处：《Chinese Chemical Letters》2022年第9期4380-4384,共5页中国化学快报（英文版）

基　　金：supported by the National Key Research and Development Program of China (No. 2020YFA0406103);National Natural Science Foundation of China (Nos. 51902217 and 21771134);National Key Research and Development Program of China(No. 2017YFA0204800);National MCF Energy R&D Program (No. 2018YFE0306105);the Suzhou Key Laboratory of Functional Nano & Soft Materials, Collaborative Innovation Center of Suzhou Nano Science & Technology;the 111 Project;Joint International Research Laboratory of Carbon-Based Functional Materials and Devices

摘　　要：Carbon dioxide electrochemical reduction(CO_(2)RR)has been recognized as an efficient way to mitigate CO_(2)emissions and alleviate the pressure on global warming and associated environmental consequences.Gold(Au)is reported as stable and active electrocatalysts to convert CO_(2)to CO at low overpotential due to its moderate adsorption strength of^(*)COOH and^(*)CO.The request for improved catalytic performance,however,is motivated by current unsatisfied catalytic selectivity because of the side hydrogen evolution reaction.In this context,the design of Au based binary catalysts that can boost CO selectivity is of great interest.In the present work,we report that Au nanoparticles can be feasibly dispersed and anchored on silicon nanowires to form Au-Si binary nanomaterials.The Au-Si may stably drive CO_(2)RR with a CO Faraday efficiency of 95.6%at−0.6 V vs.RHE in 0.5 mol/L KHCO_(3)solution.Such selectivity outperforms Au particles by up to 61%.Controlled experiments illustrate that such catalytic enhancement can chiefly be ascribed to electronic effects of binary catalysts.Theoretical calculations reveal that spontaneously produced silicon oxide may not only inhibit hydrogen evolution reaction,but also stabilize the key intermediate^(*)COOH in CO formation.

关 键 词：Gold nanoparticles Silicon nanowires ELECTROCATALYSIS Carbon dioxide reduction Noble metals 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学]