Dynamic Evolution of Active Sites in Electrocatalytic CO2 Reduction Reaction: Fundamental Understanding and Recent Progress,Advanced Functional Materials

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Dynamic Evolution of Active Sites in Electrocatalytic CO2 Reduction Reaction: Fundamental Understanding and Recent Progress
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-01-05 , DOI: 10.1002/adfm.202111193
Wenchuan Lai ₁ , Zesong Ma ₁ , Jiawei Zhang ₁ , Yuliang Yuan ₁ , Yan Qiao ₁ , Hongwen Huang _{1,

2}

Affiliation

Advancing the development of electrocatalytic CO₂ reduction reaction (CO₂RR) to address the environmental issues caused by excessive consumption of fossil fuels requires rational design of remarkable electrocatalysts, where the identification of active sites and further understanding of structure–performance relationship are the bases. However, the notable dynamic evolution often appears on the catalysts, with typical examples of Cu-based catalysts, under operating conditions, causing great difficulty in identifying the real active sites and further understanding the correlations between structure and catalytic property. In this context, understanding the dynamic evolution process of catalytically active sites during CO₂RR is of particular importance, which inspires to organize the present review. Herein, the fundamental principles of dynamic evolution in CO₂RR including thermodynamics and kinetics aspects, followed by the introduction of operando techniques employed to probe the evolution under operating conditions are first highlighted. The dynamic evolution behaviors, involving atomic rearrangement and change in chemical state, on typical catalysts are further discussed, with emphasis on the correlations between evolution behaviors and catalytic properties (activity, selectivity, and stability). The emerging CO₂ pulsed electrolysis technique that behaves promise to manipulate the dynamic evolution and future opportunities are finally discussed.

中文翻译：

电催化 CO2 还原反应中活性位点的动态演化：基本认识和最新进展

推进电催化CO ₂还原反应（CO ₂ RR）的发展，以解决化石燃料过度消耗引起的环境问题，需要合理设计卓越的电催化剂，其中活性位点的识别和结构-性能关系的进一步理解是基础. 然而，显着的动态演化往往出现在催化剂上，典型的例子是铜基催化剂，在操作条件下，很难确定真正的活性位点，也很难进一步理解结构与催化性能之间的相关性。_{在此背景下，了解 CO 2}过程中催化活性位点的动态演化过程RR 特别重要，它激发了组织本次审查的灵感。_{在此，首先强调了 CO 2} RR动态演化的基本原理，包括热力学和动力学方面，然后引入了用于探测操作条件下演化的操作技术。进一步讨论了典型催化剂上涉及原子重排和化学状态变化的动态演化行为，重点讨论了演化行为与催化性能（活性、选择性和稳定性）之间的相关性。最后讨论了新兴的 CO ₂脉冲电解技术，该技术有望控制动态演化和未来的机遇。

更新日期：2022-01-05

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