Regulating ethane and ethylene synthesis by proton corridor microenvironment for CO_(2) electrolysis  

作　　者：Xiaowen Zhang Bohua Ren Hao Li Shuxuan Liu Haoyang Xiong Silong Dong Yifan Li Dan Luo Yi Cui Guobin Wen Xin Wang 

机构地区：[1]South China Academy of Advanced Optoelectronics,International Academy of Optoelectronics at Zhaoqing,South China Normal University,Guangzhou 510006,Guangdong,China [2]Department of Chemical Engineering,Waterloo Institute for Nanotechnology,University of Waterloo,200 University Avenue West,Waterloo,Ontario N2L 3G1,Canada [3]School of Nano Technology and Nano Bionics,University of Science and Technology of China,Hefei 230026,Anhui,China [4]i-lab,Nano-X Vacuum Interconnected Workstation,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences,Suzhou 215123,Jiangsu,China [5]State Key Laboratory of Chem/Bio-Sensing and Chemometrics,Provincial Hunan Key Laboratory for Graphene Materials and Devices,College of Chemistry and Chemical Engineering,National Supercomputer Centers in Changsha,Hunan University,Changsha 410082,Hunan,China

出　　处：《Journal of Energy Chemistry》2023年第12期368-377,I0010,共11页能源化学（英文版）

基　　金：financially supported by the Outstanding Youth Project of Guangdong Natural Science Foundation (2021B1515020051);the financial support from the Basic and Applied Basic Research Foundation of Guangdong Province (2021B1515120024, 2022A1515011804)。

摘　　要：Electrocatalytic reduction of carbon dioxide is one of the most effective strategies to achieve carbon neutrality and energy sustainability.Although high-value multi-carbon products have been widely studied,limited electrocatalysts have been reported for the selective conversion of ethane.More importantly,the factors tuning the selectivity between ethane and ethylene have not been clarified.Here,Zn@Cu nanowire arrays(Zn@Cu-NWAs) catalyst is proposed to stimulate the maintenance of efficient CO_(2)-to-C_(2)H_(6) conversion at high current densities.Meanwhile,in order to investigate the factors affecting the interconversion between ethane and ethylene,the counterpart catalyst that facilitates C–C coupling to ethylene was also synthesized.Time-of-flight secondary-ion mass spectroscopy(TOF-SIMS),in-situ Raman spectroscopy,and simulation results show that Zn@Cu-NWAs can provide a localized proton corridor environment for the formation of ethane,accelerating the further proton-coupled CO_(2) reduction reaction(CO_(2)RR)kinetics.Hence,this catalyst delivered an ethane Faraday efficiency of over 65% at-1.14 V vs.RHE with a total current density of 142.3 mA/cm^(2).This work provides a new perspective on regulating the local microenvironment to modify the selectivity of multi-carbon products.

关 键 词：Proton microenvironment CO_(2)reduction C2+product Selective conversion Cu-Zn materials 

分 类 号：TQ203.2[化学工程—有机化工] TQ221