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Title: Influence of surface oxidation on ion dynamics and capacitance in porous and nonporous carbon electrodes

Abstract

Here, we investigate the influence of surface chemistry and ion confinement on capacitance and electrosorption dynamics of room-temperature ionic liquids (RTILs) in supercapacitors. Using air oxidation and vacuum annealing, we produced defunctionalized and oxygen-rich surfaces of carbide-derived carbons (CDCs) and graphene nanoplatelets (GNPs). While oxidized surfaces of porous CDCs improve capacitance and rate handling abilities of ions, defunctionalized nonporous GNPs improve charge storage densities on planar electrodes. Quasi-elastic neutron scattering (QENS) and inelastic neutron scattering (INS) probed the structure, dynamics, and orientation of RTIL ions confined in divergently functionalized pores. Oxidized, ionophilic surfaces draw ions closer to pore surfaces and enhance potential-driven ion transport during electrosorption. Molecular dynamics (MD) simulations corroborated experimental data and demonstrated the significance of surface functional groups on ion orientations, accumulation densities, and capacitance.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [2];  [1]
  1. Drexel Univ., Philadelphia, PA (United States)
  2. Vanderbilt Univ., Nashville, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1250416
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 120; Journal Issue: 16; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dyatkin, Boris, Zhang, Yu, Mamontov, Eugene, Kolesnikov, Alexander I., Cheng, Yongqiang, Meyer, III, Harry M., Cummings, Peter T., and Gogotsi, Yury G. Influence of surface oxidation on ion dynamics and capacitance in porous and nonporous carbon electrodes. United States: N. p., 2016. Web. doi:10.1021/acs.jpcc.6b01204.
Dyatkin, Boris, Zhang, Yu, Mamontov, Eugene, Kolesnikov, Alexander I., Cheng, Yongqiang, Meyer, III, Harry M., Cummings, Peter T., & Gogotsi, Yury G. Influence of surface oxidation on ion dynamics and capacitance in porous and nonporous carbon electrodes. United States. https://doi.org/10.1021/acs.jpcc.6b01204
Dyatkin, Boris, Zhang, Yu, Mamontov, Eugene, Kolesnikov, Alexander I., Cheng, Yongqiang, Meyer, III, Harry M., Cummings, Peter T., and Gogotsi, Yury G. 2016. "Influence of surface oxidation on ion dynamics and capacitance in porous and nonporous carbon electrodes". United States. https://doi.org/10.1021/acs.jpcc.6b01204. https://www.osti.gov/servlets/purl/1250416.
@article{osti_1250416,
title = {Influence of surface oxidation on ion dynamics and capacitance in porous and nonporous carbon electrodes},
author = {Dyatkin, Boris and Zhang, Yu and Mamontov, Eugene and Kolesnikov, Alexander I. and Cheng, Yongqiang and Meyer, III, Harry M. and Cummings, Peter T. and Gogotsi, Yury G.},
abstractNote = {Here, we investigate the influence of surface chemistry and ion confinement on capacitance and electrosorption dynamics of room-temperature ionic liquids (RTILs) in supercapacitors. Using air oxidation and vacuum annealing, we produced defunctionalized and oxygen-rich surfaces of carbide-derived carbons (CDCs) and graphene nanoplatelets (GNPs). While oxidized surfaces of porous CDCs improve capacitance and rate handling abilities of ions, defunctionalized nonporous GNPs improve charge storage densities on planar electrodes. Quasi-elastic neutron scattering (QENS) and inelastic neutron scattering (INS) probed the structure, dynamics, and orientation of RTIL ions confined in divergently functionalized pores. Oxidized, ionophilic surfaces draw ions closer to pore surfaces and enhance potential-driven ion transport during electrosorption. Molecular dynamics (MD) simulations corroborated experimental data and demonstrated the significance of surface functional groups on ion orientations, accumulation densities, and capacitance.},
doi = {10.1021/acs.jpcc.6b01204},
url = {https://www.osti.gov/biblio/1250416}, journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 16,
volume = 120,
place = {United States},
year = {Thu Apr 07 00:00:00 EDT 2016},
month = {Thu Apr 07 00:00:00 EDT 2016}
}

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Works referencing / citing this record:

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