School of Chemical Engineering, University of Adelaide, Adelaide, SA 5005, Australia.
Chem Soc Rev. 2015 Apr 21;44(8):2060-86. doi: 10.1039/c4cs00470a.
A fundamental change has been achieved in understanding surface electrochemistry due to the profound knowledge of the nature of electrocatalytic processes accumulated over the past several decades and to the recent technological advances in spectroscopy and high resolution imaging. Nowadays one can preferably design electrocatalysts based on the deep theoretical knowledge of electronic structures, via computer-guided engineering of the surface and (electro)chemical properties of materials, followed by the synthesis of practical materials with high performance for specific reactions. This review provides insights into both theoretical and experimental electrochemistry toward a better understanding of a series of key clean energy conversion reactions including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The emphasis of this review is on the origin of the electrocatalytic activity of nanostructured catalysts toward the aforementioned reactions by correlating the apparent electrode performance with their intrinsic electrochemical properties. Also, a rational design of electrocatalysts is proposed starting from the most fundamental aspects of the electronic structure engineering to a more practical level of nanotechnological fabrication.
由于过去几十年对电催化过程本质的深刻认识以及光谱学和高分辨率成像技术的最新进展，人们对表面电化学的理解发生了根本性的变化。如今，人们可以根据电子结构的深厚理论知识，通过计算机引导的材料表面和（电化学）性能设计，以及随后合成具有特定反应高性能的实际材料，来更好地设计电催化剂。这篇综述深入探讨了理论和实验电化学，以更好地理解一系列关键的清洁能源转换反应，包括氧还原反应（ORR）、氧析出反应（OER）和析氢反应（HER）。本综述的重点是通过将明显的电极性能与其内在电化学性质相关联，来解释纳米结构催化剂对上述反应的电催化活性的起源。此外，还从电子结构工程的最基本方面出发，提出了一种更为实用的纳米技术制造水平的电催化剂的合理设计。
