Journal article
Ionic liquid structure, dynamics, and electrosorption in carbon electrodes with bimodal pores and heterogeneous surfaces
Carbon (New York), v 129, pp 104-118
Apr 2018
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
We investigate the aggregation, diffusion, and resulting electrochemical behavior of ionic liquids inside carbon electrodes with complex pore architectures and surface chemistries. Carbide-derived carbons (CDCs) with bimodal porosities and defunctionalized or oxidized electrode surfaces served as model electrode materials. Our goal was to obtain a fundamental understanding of room-temperature ionic liquid ion orientation, mobility, and electrosorption behavior. Neat 1-octyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide confined in CDCs was studied using an integrated experimental and modeling approach, consisting of quasielastic neutron scattering, small-angle neutron scattering, X-ray pair distribution function analysis, and electrochemical measurements, which were combined with molecular dynamics simulations. Our analysis shows that surface oxygen groups increase the diffusion of confined electrolytes. Consequently, the ions become more than twice as mobile in oxygen-rich pores. Although greater self-diffusion of ions translates into higher electrochemical mobilities in oxidized pores, bulk-like behavior of ions dominates in the larger mesopores and increases the overall capacitance in defunctionalized pores. Experimental results highlight strong confinement and surface effects of carbon electrodes on electrolyte behavior, and molecular dynamics simulations yield insight into diffusion and capacitance differences in specific pore regions. We demonstrate the significance of surface defects on electrosorption dynamics of complex electrolytes in hierarchical pore architectures of supercapacitor electrodes.
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Details
- Title
- Ionic liquid structure, dynamics, and electrosorption in carbon electrodes with bimodal pores and heterogeneous surfaces
- Creators
- Boris Dyatkin - A.J. Drexel Nanomaterials Institute and the Department of Materials Science and Engineering, Drexel University, Philadelphia, PA 19104, USANaresh C Osti - Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USAYu Zhang - Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN 37235, USAHsiu-Wen Wang - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831-6110, USAEugene Mamontov - Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USAWilliam T Heller - Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USAPengfei Zhang - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831-6110, USAGernot Rother - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831-6110, USAPeter T Cummings - Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN 37235, USADavid J Wesolowski - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831-6110, USAYury Gogotsi - A.J. Drexel Nanomaterials Institute and the Department of Materials Science and Engineering, Drexel University, Philadelphia, PA 19104, USA
- Publication Details
- Carbon (New York), v 129, pp 104-118
- Publisher
- Elsevier
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering
- Web of Science ID
- WOS:000424885800013
- Scopus ID
- 2-s2.0-85037674210
- Other Identifier
- 991014969749904721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Chemistry, Physical
- Materials Science, Multidisciplinary