Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss–Type Proton Transport

Prado, Desiree Mae; Robledo, Alan; Hightower, Katherine; Jahng, Anthony; Doherty, Brian; Poling, Kayla; Tuckerman, Mark; Burda, Clemens

doi:10.1002/admi.202400508

Title: Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss–Type Proton Transport

Journal Article · 12 September 2024 · Advanced Materials Interfaces

DOI: https://doi.org/10.1002/admi.202400508 · OSTI ID:2440881

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Case Western Reserve University, Cleveland, OH (United States)
New York University, NY (United States)
New York University, NY (United States); NYU Shanghai (China)

There is an increasing demand for the development of ion-conducting electrolytes for energy storage systems. Much attention is directed toward deep eutectic solvents as potential candidates. In the search for highly conductive systems, the possibility of designing deep eutectic solvents with Grotthuss-type proton transport is widely overlooked. Herein, ethaline, a mixture of choline chloride and ethylene glycol is used in a 1:2 molar ratio, to induce a significant conductivity increase with the addition of water and sulfuric acid (H₂SO₄). The achieved breakthrough conductivity is analyzed experimentally and simulated with ab initio molecular dynamics (AIMD). At sufficient water content, an H-bonding network is formed that leads to a significant breakthrough conductivity based on H₂SO₄-derived proton transfer following the long-established Grotthuss proton transport mechanism. This result is substantiated by the positive deviation from the ideal KCl line in the Walden plot. Specifically, the data series positioned above the reference line indicates a Grotthuss mechanism in action. The AIMD simulations demonstrate proton transfer between water and ethylene glycol, supported by simulation frames captured at various times.

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Research Organization:: Case Western Reserve University, Cleveland, OH (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy of Sciences

Grant/Contract Number:: SC0019409

OSTI ID:: 2440881

Journal Information:: Advanced Materials Interfaces, Journal Name: Advanced Materials Interfaces Journal Issue: 36 Vol. 11; ISSN 2196-7350

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
Grotthuss mechanism
co-solvent
conductivity
deep eutectic solvent
proton transfer

Title: Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss–Type Proton Transport

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