Influence of Surface Oxidation on Ion Dynamics and Capacitance in Porous and Nonporous Carbon Electrodes

Boris Dyatkin; Yu Zhang; Eugene Mamontov; Alexander I. Kolesnikov; Yongqiang Cheng; Harry M. Meyer; Peter T. Cummings; Yury Gogotsi

doi:10.1021/acs.jpcc.6b01204

Influence of Surface Oxidation on Ion Dynamics and Capacitance in Porous and Nonporous Carbon Electrodes

Boris Dyatkin, Yu Zhang, Eugene Mamontov, Alexander I. Kolesnikov, Yongqiang Cheng, Harry M. Meyer, Peter T. Cummings, Yury Gogotsi

Research output: Contribution to journal › Article › peer-review

45 Scopus citations

Abstract

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.

Original language	English
Pages (from-to)	8730-8741
Number of pages	12
Journal	Journal of Physical Chemistry C
Volume	120
Issue number	16
DOIs	https://doi.org/10.1021/acs.jpcc.6b01204
State	Published - Apr 28 2016

Funding

The authors (B.D., E.M., Y.Z., P.T.C., and Y.G.) were supported by the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. B.D. was also supported by the DOE Office of Science Graduate Student Research Program (SCGSR). INS and QENS measurements (at ORNL) were made available through the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. The authors thank Luke Daemen (ORNL) for assistance with INS measurements. The authors also thank Guang Feng (HUST) and Hsiu-Wen Wang (ORNL) for helpful discussions.

Funders	Funder number
DOE Office of Science Graduate Student Research Program
SCGSR
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Huazhong University of Science and Technology

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title = "Influence of Surface Oxidation on Ion Dynamics and Capacitance in Porous and Nonporous Carbon Electrodes",

abstract = "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.",

author = "Boris Dyatkin and Yu Zhang and Eugene Mamontov and Kolesnikov, {Alexander I.} and Yongqiang Cheng and Meyer, {Harry M.} and Cummings, {Peter T.} and Yury Gogotsi",

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AU - Dyatkin, Boris

AU - Zhang, Yu

AU - Mamontov, Eugene

AU - Kolesnikov, Alexander I.

AU - Cheng, Yongqiang

AU - Meyer, Harry M.

AU - Cummings, Peter T.

AU - Gogotsi, Yury

PY - 2016/4/28

Y1 - 2016/4/28

N2 - 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.

AB - 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.

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Influence of Surface Oxidation on Ion Dynamics and Capacitance in Porous and Nonporous Carbon Electrodes

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