铜基单原子催化剂电催化还原二氧化碳的研究进展  

Research progress on electrochemical CO_(2) reduction for Cu-based singleatom catalysts

作　　者：李晓皎 于小虎 于琦 Xiaojiao Li;Xiaohu Yu;Qi Yu(School of Materials Science and Engineering,Shaanxi Key Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China;School of Chemistry and Environmental Science,Shaanxi Key Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China;Department of Chemistry and Key Laboratory of Organic Optoelectronics&Molecular Engineering of Ministry of Education,Tsinghua University,Beijing 100084,China)

机构地区：[1]School of Materials Science and Engineering,Shaanxi Key Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China [2]School of Chemistry and Environmental Science,Shaanxi Key Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China [3]Department of Chemistry and Key Laboratory of Organic Optoelectronics&Molecular Engineering of Ministry of Education,Tsinghua University,Beijing 100084,China

出　　处：《Science China Materials》2023年第10期3765-3781,共17页中国科学（材料科学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(92061109);the Natural Science Basic Research Program of Shaanxi(2021JCW-20 and 2022KJXX-18)。

摘　　要：电化学二氧化碳还原反应(CO_(2)RR)通过将CO_(2)转化为高价值化学品和燃料来降低其在大气中的浓度,是解决能源危机的重要途径.因此,合理设计高效、经济的电化学催化剂至关重要.研究发现,铜(Cu)是一种性能优越的金属催化剂,可将CO_(2)还原成碳氢化合物和醇类,尤其是C_(2+)产物.然而,Cu催化剂也存在一定问题(如过电位高和CO_(2)RR选择性差等),从而限制了其应用.近年来,单原子催化剂(SACs)因其具有高活性、高选择性和高稳定性,已成为异相催化剂领域的新兴研究前沿.本文总结了CO_(2)RR的各种铜基SACs的最新研究进展,尤其是活性位点与关键反应中间产物相互作用的调控策略.这种相互作用对于设计活性位点以及优化多电子还原步骤和提高催化性能非常重要.同时,本文还讨论了金属中心调控、铜基单原子合金催化剂、非金属SACs、串联催化剂和复合催化剂等研究前沿.最后,总结了SACs应用于CO_(2)RR的挑战与展望.Electrochemical CO_(2) reduction reaction(CO_(2)RR)is a critical route to reduce the concentration of CO_(2) in the atmosphere and solve the energy crisis by converting CO_(2) into high-value chemicals and fuels.It is therefore crucial to rationally design efficient and cost-effective electrochemical catalysts.Copper(Cu)is found to be an excellent metal catalyst that can reduce CO_(2) to hydrocarbons and alcohols,especially C_(2+)products.However,there exist some problems(such as high overpotential and poor selectivity in CO_(2)RR)that limit the application of Cu-based catalysts.In recent years,singleatom catalysts(SACs)have become an emerging research frontier in the field of heterogeneous catalysis due to their potential high activity,selectivity,and stability.Herein,the recent progress of various Cu-based SACs for CO_(2)RR has been reviewed,especially on the regulatory strategies for the interaction of the active site with key reaction intermediates.This interaction is important for designing the active site to optimize the multi-electron reduction step and improve the catalytic performance.Meanwhile,different design strategies,including the regulation of metal centers,Cu-based singleatom alloy catalysts(SAAs),non-metal SACs,tandem catalysts,and composite catalysts,have also been discussed.Finally,the current research challenges and future developments of SACs in CO_(2)RR have been summarized.

关 键 词：CO_(2)reduction reaction ELECTROCHEMICAL single-atom catalysts Cu-based reaction mechanism 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]