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Title: Relationship between pore size and reversible and irreversible immobilization of ionic liquid electrolytes in porous carbon under applied electric potential

Abstract

Transport of electrolytes in nanoporous carbon-based electrodes largely defines the function and performance of energy storage devices. Here, using molecular dynamics simulation and quasielastic neutron scattering, we investigate the microscopic dynamics of a prototypical ionic liquid electrolyte, [emim][Tf 2N], under applied electric potential in carbon materials with 6.7 nm and 1.5 nm pores. The simulations demonstrate the formation of dense layers of counter-ions near the charged surfaces, which is reversible when the polarity is reversed. In the experiment, the ions immobilized near the surface manifest themselves in the elastic scattering signal. The experimentally observed ion immobilization near the wall is fully reversible as a function of the applied electric potential in the 6.7 nm, but not in the 1.5 nm nanopores. In the latter case, remarkably, the first application of the electric potential leads to apparently irreversible immobilization of cations or anions, depending on the polarity, near the carbon pore walls. This unexpectedly demonstrates that in carbon electrode materials with the small pores, which are optimal for energy storage applications, the polarity of the electrical potential applied for the first time after the introduction of an ionic liquid electrolyte may define the decoration of the small pore walls with ionsmore » for prolonged periods of time and possibly for the lifetime of the electrode.« less

Authors:
 [1];  [2];  [3];  [1];  [4];  [3];  [5]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  3. Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  4. Univ. of Alabama, Tuscaloosa, AL (United States). Dept. of Chemical and Biological Engineering
  5. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA; Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, USA
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1328320
Alternate Identifier(s):
OSTI ID: 1420531
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 109; Journal Issue: 14; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; carbon; electrolytes; molecular dynamic

Citation Formats

Mahurin, Shannon M., Mamontov, Eugene, Thompson, Matthew W., Zhang, Pengfei, Turner, C. Heath, Cummings, Peter T., and Dai, Sheng. Relationship between pore size and reversible and irreversible immobilization of ionic liquid electrolytes in porous carbon under applied electric potential. United States: N. p., 2016. Web. doi:10.1063/1.4964130.
Mahurin, Shannon M., Mamontov, Eugene, Thompson, Matthew W., Zhang, Pengfei, Turner, C. Heath, Cummings, Peter T., & Dai, Sheng. Relationship between pore size and reversible and irreversible immobilization of ionic liquid electrolytes in porous carbon under applied electric potential. United States. doi:10.1063/1.4964130.
Mahurin, Shannon M., Mamontov, Eugene, Thompson, Matthew W., Zhang, Pengfei, Turner, C. Heath, Cummings, Peter T., and Dai, Sheng. Tue . "Relationship between pore size and reversible and irreversible immobilization of ionic liquid electrolytes in porous carbon under applied electric potential". United States. doi:10.1063/1.4964130. https://www.osti.gov/servlets/purl/1328320.
@article{osti_1328320,
title = {Relationship between pore size and reversible and irreversible immobilization of ionic liquid electrolytes in porous carbon under applied electric potential},
author = {Mahurin, Shannon M. and Mamontov, Eugene and Thompson, Matthew W. and Zhang, Pengfei and Turner, C. Heath and Cummings, Peter T. and Dai, Sheng},
abstractNote = {Transport of electrolytes in nanoporous carbon-based electrodes largely defines the function and performance of energy storage devices. Here, using molecular dynamics simulation and quasielastic neutron scattering, we investigate the microscopic dynamics of a prototypical ionic liquid electrolyte, [emim][Tf2N], under applied electric potential in carbon materials with 6.7 nm and 1.5 nm pores. The simulations demonstrate the formation of dense layers of counter-ions near the charged surfaces, which is reversible when the polarity is reversed. In the experiment, the ions immobilized near the surface manifest themselves in the elastic scattering signal. The experimentally observed ion immobilization near the wall is fully reversible as a function of the applied electric potential in the 6.7 nm, but not in the 1.5 nm nanopores. In the latter case, remarkably, the first application of the electric potential leads to apparently irreversible immobilization of cations or anions, depending on the polarity, near the carbon pore walls. This unexpectedly demonstrates that in carbon electrode materials with the small pores, which are optimal for energy storage applications, the polarity of the electrical potential applied for the first time after the introduction of an ionic liquid electrolyte may define the decoration of the small pore walls with ions for prolonged periods of time and possibly for the lifetime of the electrode.},
doi = {10.1063/1.4964130},
journal = {Applied Physics Letters},
number = 14,
volume = 109,
place = {United States},
year = {Tue Oct 04 00:00:00 EDT 2016},
month = {Tue Oct 04 00:00:00 EDT 2016}
}

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Cited by: 5 works
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Works referenced in this record:

Synthesis of Mesoporous Carbon Materials via Enhanced Hydrogen-Bonding Interaction
journal, April 2006

  • Liang, Chengdu; Dai, Sheng
  • Journal of the American Chemical Society, Vol. 128, Issue 16, p. 5316-5317
  • DOI: 10.1021/ja060242k