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Title: Computational Insights into Materials and Interfaces for Capacitive Energy Storage

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:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 7; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
Vanderbilt Univ., Nashville, TN (United States); East China Univ. of Science and Technology, Shanghai (China)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electric double layers; electrolytes; joint density functional theory; molecular simulations; porous materials; supercapacitors
OSTI Identifier:
1352692
Alternate Identifier(s):
OSTI ID: 1352693; OSTI ID: 1376438

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., 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}
}

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