Structural Self-Reconstruction of Catalysts in Electrocatalysis

作者：Hongliang Jiang, Qun He, Youkui Zhang, Li Song · 发表于：Accounts of Chemical Research · 年份：2018 · DOI：10.1021/acs.accounts.8b00449 · 被引用次数：370 · 研究领域：Electrocatalysts for Energy Conversion、Electrochemical Analysis and Applications、Molecular Junctions and Nanostructures

Recent years have witnessed significant development of electrocatalysis for clean energy and related potential technologies. The precise identification toward active sites of catalysts and the monitoring of product information are highly desirable to understand how the materials catalyze a specific electrocatalytic reaction. For a long period, the identification of active sites and the cognition of corresponding catalytic mechanisms are generally based on various ex situ characterization methods which actually could not capture dynamic structure and intermediate information during electrocatalytic processes. With recent developments of in situ and operando characterization techniques, it has been extensively observed that most of the catalysts would undergo structural self-reconstruction as a result of electro-derived oxidation or reduction process of the catalysts at a given potential, often accompanied by the increase or decrease of catalytic activity as well as the change of catalytic selectivity. In fact, such structural self-change in the catalytic process does make it difficult to identify the true catalytically active sites efficiently, thus hindering the understanding of the real catalytic mechanism. Therefore, we believe that understanding the self-reconstruction by the combination of reliable characterization techniques and theoretical calculations holds the key to rational design of advanced catalysts. In this Account, we provide in-depth insights into recent progr...