Computational Insights into Materials and Interfaces for Capacitive Energy Storage

Abstract

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 RuO2. We summarize and conclude with an outlook for the future of materials simulation and design for capacitive energy storage.

Density Functional Theory Calculations of the Quantum Capacitance of Graphene Oxide as a Supercapacitor Electrode

“…where is the double‐layer capacitance and represents the quantum capacitance . It can be predicted from Equation 1 that the total interfacial capacitance is maximum when one of the components increases to infinite, otherwise, would be smaller than either or .…”

The Constructions and Pyrolysis of 3D Kerogen Macromolecular Models: Experiments and Simulations

“…The connectivity between atoms in the molecule of the reactive force field (ReaxFF) is determined by the interatomic bond order at that time, which means the chemical bond can be broken and formed freely, so that the chemical reaction process can be obtained . The ReaxFF method has been successfully applied to reaction kinetics simulation researches, including applications of the organic micromolecular system, the polymer system, and the high energy material system .…”

2 D Materials for Electrochemical Energy Storage: Design, Preparation, and Application

“…Reasonable theoretical simulation is an effective way to analyze the structures andp roperties of 2D materials and guide their design and exploitation. [17] Concretely,c omputational investigationsc an be used for mechanistic study and for screening of 2D materials in fields related to electrochemical energy storage.…”