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

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 wit...

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Main Authors: Desiree Mae Prado, Alan Robledo, Katherine Hightower, Anthony Jahng, Brian Doherty, Kayla Poling, Mark Tuckerman, Clemens Burda
Format: Article
Language:English
Published: Wiley-VCH 2024-12-01
Series:Advanced Materials Interfaces
Subjects:
Online Access:https://doi.org/10.1002/admi.202400508
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author Desiree Mae Prado
Alan Robledo
Katherine Hightower
Anthony Jahng
Brian Doherty
Kayla Poling
Mark Tuckerman
Clemens Burda
author_facet Desiree Mae Prado
Alan Robledo
Katherine Hightower
Anthony Jahng
Brian Doherty
Kayla Poling
Mark Tuckerman
Clemens Burda
author_sort Desiree Mae Prado
collection DOAJ
description 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.
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publishDate 2024-12-01
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series Advanced Materials Interfaces
spelling doaj-art-e8cff1bbb6da4d57be9a21e556d27e502024-12-19T12:52:15ZengWiley-VCHAdvanced Materials Interfaces2196-73502024-12-011136n/an/a10.1002/admi.202400508Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton TransportDesiree Mae Prado0Alan Robledo1Katherine Hightower2Anthony Jahng3Brian Doherty4Kayla Poling5Mark Tuckerman6Clemens Burda7Department of Chemistry Case Western Reserve University Cleveland OH 44106 USADepartment of Chemistry New York University New York NY 10003 USADepartment of Chemistry New York University New York NY 10003 USADepartment of Chemistry Case Western Reserve University Cleveland OH 44106 USADepartment of Chemistry New York University New York NY 10003 USADepartment of Chemistry Case Western Reserve University Cleveland OH 44106 USADepartment of Chemistry New York University New York NY 10003 USADepartment of Chemistry Case Western Reserve University Cleveland OH 44106 USAAbstract 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.https://doi.org/10.1002/admi.202400508conductivityco‐solventdeep eutectic solventGrotthuss mechanismproton transfer
spellingShingle Desiree Mae Prado
Alan Robledo
Katherine Hightower
Anthony Jahng
Brian Doherty
Kayla Poling
Mark Tuckerman
Clemens Burda
Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
Advanced Materials Interfaces
conductivity
co‐solvent
deep eutectic solvent
Grotthuss mechanism
proton transfer
title Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
title_full Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
title_fullStr Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
title_full_unstemmed Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
title_short Breakthrough Conductivity Enhancement in Deep Eutectic Solvents via Grotthuss‐Type Proton Transport
title_sort breakthrough conductivity enhancement in deep eutectic solvents via grotthuss type proton transport
topic conductivity
co‐solvent
deep eutectic solvent
Grotthuss mechanism
proton transfer
url https://doi.org/10.1002/admi.202400508
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