赝电容超级电容器的理论模拟研究进展

doi:10.19799/j.cnki.2095-4239.2025.0519

摘要/Abstract

摘要：

赝电容器兼具高能量密度与高功率密度的独特优势，在储能领域备受关注。过去十年间，研究人员对赝电容材料的研发与性能提升取得了显著进展。然而，赝电容界面的复杂性和快速充放电特性使得传统实验表征难以全面揭示其离子传输与电荷转移机制，如何全面解析赝电容的微观机理，依然是该领域的难点问题。本综述系统梳理了赝电容理论的发展历程，重点厘清了其与双电层电容及电池行为的本质区别。基于近期的研究进展，深入探讨了理论模拟方法在赝电容机理研究中的关键作用，包括第一性原理计算、隐式溶剂化模型、分子动力学模拟、从头算分子动力学、连续介质输运模型以及多尺度耦合方法的应用。这些模拟技术为解析赝电容材料的界面反应动力学、离子传输机制及结构性能关系提供了重要理论支撑，为高性能赝电容器的设计指明了方向。

关键词: 赝电容, 第一性原理, 分子动力学, 隐式溶剂化模型, 多尺度耦合

Abstract:

Pseudocapacitors are of great interest for energy storage applications due to their exceptional ability to deliver both high energy and power densities. Over the past decade, significant advances have been achieved in the development and performance enhancement of pseudocapacitive materials. However, the inherent complexity of pseudocapacitive interfaces and their rapid charge-discharge characteristics pose significant challenges for conventional experimental techniques to fully elucidate the coupled ion transport and charge transfer mechanisms. A comprehensive understanding of the microscopic processes underlying pseudocapacitance remains a critical challenge in this field. This review systematically traces the evolution of pseudocapacitance theory, emphasizing the fundamental distinctions between pseudocapacitance, electric double-layer capacitance, and battery-type behavior. By integrating recent advances in computational modeling, the review critically assesses the crucial role of computational simulations in elucidating pseudocapacitive mechanisms. Key methodologies discussed include first-principles calculations, molecular dynamics simulations, implicit solvation models, ab initio molecular dynamics, continuum transport models, and multiscale simulation strategies. These simulation techniques provide vital theoretical insights into interfacial reaction kinetics, ion transport mechanisms, and structure-property relationships, thereby guiding the rational design of high-performance pseudocapacitors.

Key words: Pseudocapacitors, First-principles, Molecular dynamics, Implicit solvation model, Multiscale simulation strategies

邢甫旭, 覃琪, 王龙康, 黎裕冰, 徐帅凯, 莫唐明. 赝电容超级电容器的理论模拟研究进展[J]. 储能科学与技术, doi: 10.19799/j.cnki.2095-4239.2025.0519.

Fuxu XING, Qi QIN, Longka WANG, Yubing LI, Shuaikai XU, Tangming MO. Recent advances in theory and computational simulation of pseudocapacitors[J]. Energy Storage Science and Technology, doi: 10.19799/j.cnki.2095-4239.2025.0519.

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