Open AccessComputational Insights into Materials and Interfaces for Capacitive Energy Storage
Author(s) -
Zhan Cheng,
Lian Cheng,
Zhang Yu,
Thompson Matthew W.,
Xie Yu,
Wu Jianzhong,
Kent Paul R. C.,
Cummings Peter T.,
Jiang Deen,
Wesolowski David J.
Publication year - 2017
Publication title -
advanced science
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.388
H-Index - 100
ISSN - 2198-3844
DOI - 10.1002/advs.201700059
Subject(s) - pseudocapacitor , supercapacitor , capacitance , density functional theory , energy storage , pseudocapacitance , electrolyte , materials science , capacitive sensing , capacitor , dielectric , nanotechnology , electric double layer capacitor , electrode , computer science , optoelectronics , electrical engineering , chemistry , physics , power (physics) , computational chemistry , thermodynamics , engineering , voltage , operating system
Supercapacitors such as electric double‐layer capacitors (EDLCs) and pseudocapacitors are becoming increasingly important in the field of electrical energy storage. Theoretical study of energy storage in EDLCs focuses on solving for the electric double‐layer structure in different electrode geometries and electrolyte components, which can be achieved by molecular simulations such as classical molecular dynamics (MD), classical density functional theory (classical DFT), and Monte‐Carlo (MC) methods. In recent years, combining first‐principles and classical simulations to investigate the carbon‐based EDLCs has shed light on the importance of quantum capacitance in graphene‐like 2D systems. More recently, the development of joint density functional theory (JDFT) enables self‐consistent electronic‐structure calculation for an electrode being solvated by an electrolyte. In contrast with the large amount of theoretical and computational effort on EDLCs, theoretical understanding of pseudocapacitance is very limited. In this review, we first introduce popular modeling methods and then focus on several important aspects of EDLCs including nanoconfinement, quantum capacitance, dielectric screening, and novel 2D electrode design; we also briefly touch upon pseudocapactive mechanism in RuO 2 . We summarize and conclude with an outlook for the future of materials simulation and design for capacitive energy storage.