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

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

doi:10.1021/acs.jpcc.6b01204

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

Journal Article · Thu Apr 07 04:00:00 EDT 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b01204· OSTI ID:1250416

Dyatkin, Boris ^[1]; Zhang, Yu ^[2]; Mamontov, Eugene ^[3]; Kolesnikov, Alexander I. ^[3]; Cheng, Yongqiang ^[3]; Meyer, III, Harry M. ^[3]; Cummings, Peter T. ^[2]; Gogotsi, Yury G. ^[1]

Drexel Univ., Philadelphia, PA (United States)
Vanderbilt Univ., Nashville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1250416

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 16 Vol. 120; ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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