Progress of mechanistic pathways involved in electrochemical CO_(2)reduction  

作　　者：Jing-Wen DuanMu Xue-Peng Yang Fei-Yue Gao Masoud Atapour Min-Rui Gao 

机构地区：[1]Division of Nanomaterials&Chemistry,Hefei National Laboratory for Physical Sciences at the Microscale,Department of Chemistry,University of Science and Technology of China,Hefei 230026,Anhui,China [2]School of Materials Science and Engineering,Anhui University,Hefei 230601,Anhui,China [3]Department of Materials Engineering,Isfahan University of Technology,Isfahan 84156-83111,Iran

出　　处：《Journal of Energy Chemistry》2025年第3期745-767,共23页能源化学(英文版)

基　　金：financially supported by the National Natural Science Foundation of China(Grants 22225901,21975237 and 51702312);the Fundamental Research Funds for the Central Universities(Grant WK2340000101);the USTC Research Funds of the Double First-Class Initiative(Grant YD2340002007 and YD9990002017);the Open Funds of the State Key Laboratory of Rare Earth Resource Utilization(Grant RERU2022007);the China Postdoctoral Science Foundation(Grants 2023M733371,2024M750006 and 2023T160617);Postdoctoral Fellowship Program(Grade C)of China Postdoctoral Science Foundation(GZC20230008);the Natural Science Foundation Youth Project of Anhui Province(2408085QB065);the Postdoctoral Research Funding Project of Anhui Province(2023B727)。

摘　　要：The electrochemical reduction of carbon dioxide(CO_(2))into value-added chemicals and fuels has been extensively studied as a promising strategy for mitigating environmental issues and achieving sustainable energy conversion.Substantial efforts have been made to improve the understanding of CO_(2)reduction reaction(CO_(2)RR)mechanisms by computational and spectroscopic studies.An in-depth understanding of CO_(2)RR mechanism can provide the guidance and criteria for designing high-efficiency catalysts,and hence,steering CO_(2)RR to desired products.This review systematically discusses the formation mechanisms and reaction pathways of various CO_(2)RR products,including C_(1)products(CO,HCOOH,and CH_(4)),C_(2)products(C_(2)H_(4),C_(2)H_(5)OH,and CH_(3)COOH),and C_(3+)products(C_(3)H_(6),C_(3)H_(7)OH,and others).The reaction pathways are elucidated by analyzing the adsorption behavior,energy barriers,and intermediate coupling steps involved in the generation of each product.Particular emphasis is placed on the key intermediates,such as^(*)OCHO,^(*)COOH,^(*)CO,^(*)OCCOH,and^(*)CCO,which play crucial roles in determining the product selectivity.The effects of catalyst composition,morphology,and electronic structure on the adsorption and activation of these intermediates are also discussed.Moreover,advanced characterization techniques,including in-situ spectroscopy and isotopic labeling experiments,are highlighted for their contributions to unraveling the reaction mechanisms.The review aims to provide critical insights to reveal the activity-determining para meters and underlying CO_(2)RR mechanisms,which will guide the rational design of next-generation electrocatalysts for selective CO^(2)RR towards high-value products.

关 键 词：CO_(2)reduction reaction Reaction pathways Faradaic efficiency Catalytic mechanism Cataly ststructure 

分 类 号：O643.3[理学—物理化学]