Electrochemical energy conversion has emerged as one of the most promising approaches to alleviate the issues of energy shortage and environmental pollution by converting small molecules into higher value products in a sustainable way. Practical applications of this technology are limited by the development of electrocatalysts with low cost, high activity, and long durability. Huge advances have been achieved in electrocatalyst discovery during the past decades, and computational means have played an irreplaceable role. Inspired by this, we introduce and discuss “how computations accelerate electrocatalyst discovery” in this review, from the aspects of providing insights and guidelines. By using some typical examples, the advances of theoretical investigations aimed at identifying the active sites and understanding the reaction mechanisms and activity origin are first summarized. Then, an overview of the design principles and screening strategies for superior electrocatalysts is highlighted. We close by outlining the future perspectives in this field.

通过以可持续的方式将小分子转化为更高价值的产品，电化学能量转换已成为缓解能源短缺和环境污染问题的最有希望的方法之一。该技术的实际应用受限于低成本、高活性和长耐久性的电催化剂的开发。在过去的几十年里，电催化剂的发现取得了巨大的进步，计算手段发挥了不可替代的作用。受此启发，我们在这篇综述中从提供见解和指导的方面介绍和讨论了“计算如何加速电催化剂的发现”。通过一些典型的例子，首先总结了旨在识别活性位点并了解反应机理和活性起源的理论研究进展。然后，重点概述了优质电催化剂的设计原则和筛选策略。最后，我们概述了该领域的未来前景。