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电还原反应中催化剂的结构重构:识别、理解与调控

Structural Reconstruction of Catalysts in Electroreduction Reaction: Identifying, Understanding, and Manipulating.

作者信息

Wang Wenbin, Duan Junyuan, Liu Youwen, Zhai Tianyou

机构信息

State Key Laboratory of Materials Processing and Die & Mould Technology, and School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, P. R. China.

出版信息

Adv Mater. 2022 Dec;34(52):e2110699. doi: 10.1002/adma.202110699. Epub 2022 Aug 18.

DOI:10.1002/adma.202110699
PMID:35460124
Abstract

Electroreduction transformation of small molecules (CO , N , and H O) into chemical feedstocks offers a promising approach to eliminate carbon emissions and harness renewable energy. Most cathodic catalysts often undergo structural transformation under operating electroreduction conditions. These structural reconstructions are reflected in changes in their catalytic activity. In-depth understanding of the change of active sites and influence parameters of reconstruction behaviors is an essential precondition for the design of highly efficient catalysts. Despite the previous achievements, comprehensive insight toward the structural evolution mechanism in cathodic catalysts, compared to anode ones, under reaction conditions is still lacking. Herein, an overview of structural reconstruction for cathodic catalysts in terms of fundamental mechanisms, reconstruction process, advanced characterizations, and influencing parameters is provided. On this basis, the typical strategies for manipulating the structural reconfiguration of catalysts are also explicitly discussed from the catalyst structure and working environment. By delivering the mechanism, strategies, insights, and techniques, this review will provide a comprehensive understanding of the structural reconstruction of cathodic catalysts in electroreduction reactions and future guidelines for their rational development.

摘要

将小分子(CO₂、N₂和H₂O)电还原转化为化学原料为消除碳排放和利用可再生能源提供了一种很有前景的方法。大多数阴极催化剂在运行的电还原条件下常常会发生结构转变。这些结构重构反映在其催化活性的变化上。深入了解活性位点的变化以及重构行为的影响参数是设计高效催化剂的必要前提。尽管有先前的研究成果,但相比于阳极催化剂,在反应条件下对阴极催化剂结构演变机制仍缺乏全面的认识。在此,本文从基本机制、重构过程、先进表征方法以及影响参数等方面对阴极催化剂的结构重构进行了综述。在此基础上,还从催化剂结构和工作环境方面明确讨论了操控催化剂结构重新配置的典型策略。通过阐述机制、策略、见解和技术,本综述将提供对电还原反应中阴极催化剂结构重构的全面理解以及其合理开发的未来指导方针。

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