Structural Anomalies and Electronic Properties of an Ionic Liquid under Nanoscale Confinement
Name
1698282.pdf
Description
Accepted version
Size
578.68 KB
Format
Adobe PDF
Checksum (MD5)
4866300e8040e7d487c5c41c27c0eb93
Author(s)
Pham, Tuan Anh
Coulthard, Riley M
Zobel, Mirijam
Maiti, Amitesh
Buchsbaum, Steven F
Loeb, Colin
Campbell, Patrick G
Plata, Desirée L
Wood, Brandon C
Fornasiero, Francesco
Date Issued
July 2020
Journal
Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
Pham, Tuan Anh, Coulthard, Riley M, Zobel, Mirijam, Maiti, Amitesh, Buchsbaum, Steven F et al. 2020. "Structural Anomalies and Electronic Properties of an Ionic Liquid under Nanoscale Confinement." Journal of Physical Chemistry Letters, 11 (15).
Version
Author's final manuscript
Abstract
Ionic liquids (ILs) promise far greater electrochemical performance compared to aqueous systems, yet key physicochemical properties governing their assembly at interfaces within commonly used graphitic nanopores remain poorly understood. In this work, we combine synchrotron X-ray scattering with first-principles molecular dynamics simulations to unravel key structural characteristics of 1-alkyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([TFSI]-) ionic liquids confined in carbon slit pores. X-ray scattering reveals selective pore filling due to size exclusion, while filled pores exhibit disruption in the IL intermolecular structure, the extent of which increases for narrower slit pores. First-principles simulations corroborate this finding and quantitatively describe how perturbations in the local IL structure, particularly the hydrogen-bond network, depend strongly on the degree of confinement. Despite significant deviations in structure under confinement, electrochemical stability remains intact, which is important for energy storage based on nanoporous carbon electrodes (e.g., supercapacitors).
MIT Department
Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
Terms of Use
Creative Commons Attribution-Noncommercial-Share Alike
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/ACS.JPCLETT.0C01810
