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Title: Cation Molecular Structure Affects Mobility and Transport of Electrolytes in Porous Carbons

Journal Article · · Journal of the Electrochemical Society
DOI:https://doi.org/10.1149/2.0131904jes· OSTI ID:1505315
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [1];  [1]; ORCiD logo [5]; ORCiD logo [5];  [3];  [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  2. Drexel Univ., Philadelphia, PA (United States). A. J. Drexel Nanotechnology Inst., Dept. of Materials Science and Engineering
  3. Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering
  4. Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab., ISIS Neutron Source Pulsed Neutron and Muon Source
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division
+ Show Author Affiliations

We examined the electrosorption and ion dynamics of imidazolium-based room temperature ionic liquids (RTILs) having short (3-carbon, C3mim+) and long (12-carbon, C12mim+) cations, that is, 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C3mimTFSI) and 1-dodecyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C12mimTFSI), confined in ordered mesoporous carbon (OMC) and analyzed the influence of the cation alkyl chain length on the ion dynamics and the capacitive behavior using electrochemical measurements together with quasi-elastic neutron scattering (QENS) observations and classical density functional theory (cDFT) computations. Electrochemical tests highlighted the significant influence of specific applied potentials on accumulated charge storage densities and on the limits of saturation of larger electrolytes in the pores. Computational analyses corroborated these findings and predicted a 16% increase in the capacitance of the smaller-cation electrolyte under high applied potentials. However, QENS experiments revealed a behavior of decoupling of alkyl chain dynamics from the ring in electrolytes with larger ions. cDFT calculations identified density spikes for C12mim+ away from the pore walls to further corroborate this unique behavior. Here, our insights into chain length-dependent dynamics and electrosorption in complex electrolyte-electrode systems deepen fundamental understanding of confined RTIL electrolyte behavior in the porous carbon electrodes.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC05-00OR22725; DGE-1326120
OSTI ID:
1505315
Journal Information:
Journal of the Electrochemical Society, Vol. 166, Issue 4; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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Cited By (4)

Microscopic dynamics in room-temperature ionic liquids confined in materials for supercapacitor applications journal January 2020
Side-chain effects on the capacitive behaviour of ionic liquids in microporous electrodes journal August 2019
Algorithm for Assessing the Convergence of a Cyclic Voltammetry to Its Limit Cycle journal January 2019
Side-chain effects on the capacitive behaviour of ionic liquids in microporous electrodes text January 2019

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