Computational Insights into Charge Storage Mechanisms of Supercapacitors

Abstract

Computational modeling methods, including molecular dynamics (MD) and Monte Carlo (MC) simulations, and density functional theory (DFT), are receiving booming interests for exploring charge storage mechanisms of electrochemical energy storage devices. These methods can effectively be used to obtain molecular scale local information or provide clear explanations for novel experimental findings that cannot be directly interpreted through experimental investigations. This short review is dedicated to emphasizing recent advances in computational simulation methods for exploring the charge storage mechanisms in typical nanoscale materials, such as nanoporous carbon materials, 2D MXene materials, and metal-organic framework electrodes. Beyond a better understanding of charge storage mechanisms and experimental observations, fast and accurate enough models would be helpful to provide theoretical guidance and experimental basis for the design of new high-performance electrochemical energy storage devices.

Mechanisms of Porous Carbon‐based Supercapacitors

“…With the development of the basic theory of electrochemical energy storage and the improvements in computational methodology and capabilities, computational modeling methods, for instance, molecular dynamics (MD), Monte Carlo (MC), and DFT, have been increasingly applied to explore the energy storage mechanism of porous electrode materials on the nano/micro scale [134] . These calculation techniques can accurately describe the interactions between the electrode/electrolyte interface during the charge and discharge process on the molecular scale or provide clear theoretical explanations for experiments that are difficult to implement [135,136] .…”

Perspectives on Working Voltage of Aqueous Supercapacitors

“…[3][4][5] The development of electrochemical energy storage materials and technologies have always been the focus of the energy storage application fields, including supercapacitors (SC) and batteries. [6][7][8][9][10] In the meantime, a bank of brilliant researchers have emerged and made tremendous contributions to developing high-performance energy storage materials. However, for the scientific community, the hot research fields are double-edged sword, as some fresh researchers do not grasp partial basic theories accurately, resulting in a few experimental conclusions and performance evaluation are controversial, and even obviously unreasonable phenomena occurs.…”

3D-Printed highly stretchable conducting polymer electrodes for flexible supercapacitors

“…8,9 As one of the most mainstream personalized electronics, supercapacitors with intriguing characteristics of not only high-power density, and fast rates of charge-discharge but also long cycling lifetimes, are regarded as promising smart and portable electronics. [10][11][12] A key challenge for designing an independent exible and stretchable supercapacitor is developing stretchable electrodes that can maintain structural integrity during repeated severe deformations that is beyond what is possible with rigid conventional devices. [13][14][15][16][17][18] Currently, several types of conventional strategies have been proposed to achieve stretchable electrodes.…”