电容存储设备允许快速充电和放电循环,使它们成为高功率应用电池的完美补充。许多材料在与离子溶液接触时显示出令人感兴趣的电容特性,尽管它们的结构和(表面)反应性非常不同。其中,纳米碳是最重要的实际应用,但是最近出现了许多纳米材料,如导电金属有机框架,2D材质,和各种各样的金属氧化物。这些异质和复杂的电极材料难以用常规方法建模。然而,计算方法的发展,机器学习技术的结合,现在,高性能计算的不断增长的能力使我们能够解决这些类型的系统。在这篇评论中,我们总结了目前在这个方向上的努力。我们表明,根据材料的性质和充电机制,不同的方法,或它们的组合,可以提供对相互作用的理想原子尺度的洞察力。我们主要关注两个重要方面:(一)离子在复杂纳米多孔材料中的吸附研究,这需要将恒定电位分子动力学扩展到多组分系统,和(Ii)伪电容器中法拉第过程的表征,这涉及使用基于电子结构的方法。我们还讨论了最近开发的仿真方法将如何在双层电容器和伪电容器之间建立桥接,以用于未来的高功率电力存储设备。
Capacitive storage devices allow for fast charge and discharge cycles, making them the perfect complements to batteries for high power applications. Many materials display interesting capacitive properties when they are put in contact with ionic solutions despite their very different structures and (surface) reactivity. Among them, nanocarbons are the most important for practical applications, but many nanomaterials have recently emerged, such as conductive metal-organic frameworks, 2D materials, and a wide variety of metal oxides. These heterogeneous and complex electrode materials are difficult to model with conventional approaches. However, the development of computational methods, the incorporation of machine learning techniques, and the increasing power in high performance computing now allow us to tackle these types of systems. In this Review, we summarize the current efforts in this direction. We show that depending on the nature of the materials and of the charging mechanisms, different methods, or combinations of them, can provide desirable atomic-scale insight on the interactions at play. We mainly focus on two important aspects: (i) the study of ion adsorption in complex nanoporous materials, which require the extension of constant potential molecular dynamics to multicomponent systems, and (ii) the characterization of Faradaic processes in pseudocapacitors, that involves the use of electronic structure-based methods. We also discuss how recently developed simulation methods will allow bridges to be made between double-layer capacitors and pseudocapacitors for future high power electricity storage devices.