Document Type
Article
Publication Date
9-12-2024
Abstract
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.
Keywords
co-solvent, conductivity, deep eutectic solvent, grotthuss mechanism, proton transfer
Language
English
Publication Title
Advanced Materials Interfaces
Grant
DE‐SC0019409
Rights
© 2024 The Author(s). This is an Open Access work distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/) which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Creative Commons License
This work is licensed under a Creative Commons Attribution 4.0 International License.
Recommended Citation
D. M. Prado, A. Robledo, K. Hightower, A. Jahng, B. Doherty, K. Poling, M. Tuckerman, C. Burda, Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss-Type Proton Transport. Adv. Mater. Interfaces 2024, 11, 2400508. https://doi.org/10.1002/admi.202400508
Manuscript Version
Final Publisher Version