Guo Zhongyuan, Wang Tianyi, Xu Jiang, Cao Ang, Li Hao
College of Environmental and Resource Sciences, Zhejiang University, Hangzhou, 310058, China.
WPI-Advanced Institute for Materials Research (AIMR), Tohoku University, Sendai, 980-8577, Japan.
Chem Commun (Camb). 2024 Dec 3;60(97):14346-14359. doi: 10.1039/d4cc03875d.
Electrocatalysis is key to realizing a sustainable future for our society. However, the complex interface between electrocatalysts and electrolytes presents an ongoing challenge in electrocatalysis, hindering the accurate identification of effective/authentic structure-activity relationships and determination of favourable reaction mechanisms. Surface coverage and reconstruction analyses of electrocatalysts are important to address each conjecture and/or conflicting viewpoint on surface-active phases and their corresponding electrocatalytic origin, , so-called structure-activity relationships. In this review, we emphasize the importance of surface states in electrocatalysis experimentally and theoretically, providing guidelines for research practices in discovering promising electrocatalysts. Then, we summarize some recent progress of how surface states determine the adsorption strengths and reaction mechanisms of occurring electrocatalytic reactions, exemplified in the electrochemical oxygen evolution reaction, oxygen reduction reaction, nitrogen reduction reaction, CO reduction reaction, CO and N co-reductions, and hydrogen evolution reaction. Finally, the review proposes deep insights into the study of surface states, their efficient building and the application of surface Pourbaix diagrams. This review will accelerate the development of electrocatalysts and electrocatalysis theory by arousing broad consensus on the significance of surface states.
电催化对于实现我们社会的可持续未来至关重要。然而，电催化剂与电解质之间复杂的界面给电催化带来了持续的挑战，阻碍了对有效/真实结构-活性关系的准确识别以及有利反应机制的确定。电催化剂的表面覆盖和重构分析对于解决关于表面活性相及其相应电催化起源（即所谓的结构-活性关系）的每一个推测和/或相互矛盾的观点都很重要。在这篇综述中，我们从实验和理论上强调了表面态在电催化中的重要性，为发现有前景的电催化剂的研究实践提供指导方针。然后，我们总结了表面态如何决定发生的电催化反应的吸附强度和反应机制的一些最新进展，以电化学析氧反应、氧还原反应、氮还原反应、CO还原反应、CO和N共还原反应以及析氢反应为例进行说明。最后，该综述对表面态的研究、其有效构建以及表面Pourbaix图的应用提出了深刻见解。这篇综述将通过引起对表面态重要性的广泛共识来加速电催化剂和电催化理论的发展。
