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Title: 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 RuO 2. We summarize and conclude with an outlook for the future of materials simulation and design for capacitive energy storage.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [6];  [3];  [1];  [7]
  1. Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering; East China Univ. of Science and Technology, Shanghai (China). State Key Lab. of Chemical Engineering
  3. Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  5. Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences. Computer Science and Mathematics Division
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of California, Riverside, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1352692
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Resource Type:
Journal Article: Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 7; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electric double layers; electrolytes; joint density functional theory; molecular simulations; porous materials; supercapacitors

Citation Formats

Zhan, Cheng, Lian, Cheng, Zhang, Yu, Thompson, Matthew W., Xie, Yu, Wu, Jianzhong, Kent, Paul R. C., Cummings, Peter T., Jiang, De-en, and Wesolowski, David J. Computational Insights into Materials and Interfaces for Capacitive Energy Storage. United States: N. p., 2017. Web. doi:10.1002/advs.201700059.
Zhan, Cheng, Lian, Cheng, Zhang, Yu, Thompson, Matthew W., Xie, Yu, Wu, Jianzhong, Kent, Paul R. C., Cummings, Peter T., Jiang, De-en, & Wesolowski, David J. Computational Insights into Materials and Interfaces for Capacitive Energy Storage. United States. doi:10.1002/advs.201700059.
Zhan, Cheng, Lian, Cheng, Zhang, Yu, Thompson, Matthew W., Xie, Yu, Wu, Jianzhong, Kent, Paul R. C., Cummings, Peter T., Jiang, De-en, and Wesolowski, David J. 2017. "Computational Insights into Materials and Interfaces for Capacitive Energy Storage". United States. doi:10.1002/advs.201700059.
@article{osti_1352692,
title = {Computational Insights into Materials and Interfaces for Capacitive Energy Storage},
author = {Zhan, Cheng and Lian, Cheng and Zhang, Yu and Thompson, Matthew W. and Xie, Yu and Wu, Jianzhong and Kent, Paul R. C. and Cummings, Peter T. and Jiang, De-en and Wesolowski, David J.},
abstractNote = {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.},
doi = {10.1002/advs.201700059},
journal = {Advanced Science},
number = 7,
volume = 4,
place = {United States},
year = 2017,
month = 4
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/advs.201700059

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  • 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 theorymore » (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.« less
  • Carbon materials have attracted intense interests as electrode materials for electrochemical capacitors, because of their high surface area, electrical conductivity, chemical stability and low cost. Activated carbons produced by different activation processes from various precursors are the most widely used electrodes. Recently, with the rapid growth of nanotechnology, nanostructured electrode materials, such as carbon nanotubes and template-synthesized porous carbons have been developed. Their unique electrical properties and well controlled pore sizes and structures facilitate fast ion and electron transportation. In order to further improve the power and energy densities of the capacitors, carbon-based composites combining electrical double layer capacitors (EDLC)-capacitancemore » and pseudo-capacitance have been explored. They show not only enhanced capacitance, but as well good cyclability. In this review, recent progresses on carbon-based electrode materials are summarized, including activated carbons, carbon nanotubes, and template-synthesized porous carbons, in particular mesoporous carbons. Their advantages and disadvantages as electrochemical capacitors are discussed. At the end of this review, the future trends of electrochemical capacitors with high energy and power are proposed.« less