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Structural anomalies and electronic properties of an ionic liquid under nanoscale confinement

DOI: 10.1021/acs.jpclett.0c01810 DOI Help

Authors: Tuan Anh Pham (Lawrence Livermore National Laboratory) , Riley M. Coulthard (Lawrence Livermore National Laboratory; Yale University) , Mirijam Zobel (University of Bayreuth) , Amitesh Maiti (Lawrence Livermore National Laboratory) , Steven F. Buchsbaum (Lawrence Livermore National Laboratory) , Colin Loeb (Lawrence Livermore National Laboratory) , Patrick G. Campbell (Lawrence Livermore National Laboratory) , Desiree Louise Plata (MIT) , Brandon C. Wood (Lawrence Livermore National Laboratory) , Francesco Fornasiero (Lawrence Livermore National Laboratory) , Eric R. Meshot (Lawrence Livermore National Laboratory)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: The Journal Of Physical Chemistry Letters

State: Published (Approved)
Published: July 2020
Diamond Proposal Number(s): 20578

Abstract: Ionic liquids 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 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).

Journal Keywords: Anions; Quantum confinement; Cations; Aerogels; Ions

Subject Areas: Chemistry, Materials, Energy

Instruments: I15-Extreme Conditions

Other Facilities: Advanced Light Source

Added On: 13/07/2020 10:01

Discipline Tags:

Energy Storage Energy Molecular Physics Physics Physical Chemistry Energy Materials Chemistry Materials Science Nanoscience/Nanotechnology

Technical Tags:

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