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Negating the interfacial resistance between solid and liquid electrolytes for next-generation lithium batteries

Negating the interfacial resistance between solid and liquid electrolytes for next-generation lithium batteries
Negating the interfacial resistance between solid and liquid electrolytes for next-generation lithium batteries
The combination of solid and liquid electrolytes enables the development of safe and high-energy batteries where the solid electrolyte acts as a protective barrier for a high-energy lithium metal anode, while the liquid electrolyte maintains facile electrochemical reactions with the cathode. However, the contact region between the solid and liquid electrolytes is associated with a very high resistance, which severely limits the specific energy that can be practically delivered. In this work, we demonstrate a suitable approach to virtually suppress such interfacial resistance. Using a NASICON-type solid electrolyte in a variety of liquid electrolytes (ethers, DMSO, acetonitrile, ionic liquids, etc.), we show that the addition of water as electrolyte additive decreases the interfacial resistance from >100 Ω cm2 to a negligible value (<5 Ω cm2). XPS measurements reveal that the composition of the solid–liquid electrolyte interphase is very similar in wet and dry liquid electrolytes, and thus the suppression of the associated resistance is tentatively ascribed to a plasticizer or preferential ion solvation effect of water, or to a change in the interphase morphology or porosity caused by water. Our simple estimates show that the improvement in the solid–liquid electrolyte interphase resistance observed here could translate to an enhancement of 15–22% in the practical energy density of a Li–S or Li–O2 battery and improvements in the roundtrip efficiency of 21–28 percentage points.
electrolyte additives, lithium metal batteries, lithium-ion transport, solid-liquid electrolyte interphases, solid-liquid hybrid electrolytes
1944-8244
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Padmanabhan, Vivek
edf1af56-581e-4653-9887-b98a99c0e314
Meddings, Nina
3018b390-3284-4da0-a9c6-4be738803717
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Padmanabhan, Vivek
edf1af56-581e-4653-9887-b98a99c0e314
Meddings, Nina
3018b390-3284-4da0-a9c6-4be738803717

Garcia-Araez, Nuria, Padmanabhan, Vivek and Meddings, Nina (2021) Negating the interfacial resistance between solid and liquid electrolytes for next-generation lithium batteries. ACS Applied Materials & Interfaces. (doi:10.1021/acsami.1c17247).

Record type: Article

Abstract

The combination of solid and liquid electrolytes enables the development of safe and high-energy batteries where the solid electrolyte acts as a protective barrier for a high-energy lithium metal anode, while the liquid electrolyte maintains facile electrochemical reactions with the cathode. However, the contact region between the solid and liquid electrolytes is associated with a very high resistance, which severely limits the specific energy that can be practically delivered. In this work, we demonstrate a suitable approach to virtually suppress such interfacial resistance. Using a NASICON-type solid electrolyte in a variety of liquid electrolytes (ethers, DMSO, acetonitrile, ionic liquids, etc.), we show that the addition of water as electrolyte additive decreases the interfacial resistance from >100 Ω cm2 to a negligible value (<5 Ω cm2). XPS measurements reveal that the composition of the solid–liquid electrolyte interphase is very similar in wet and dry liquid electrolytes, and thus the suppression of the associated resistance is tentatively ascribed to a plasticizer or preferential ion solvation effect of water, or to a change in the interphase morphology or porosity caused by water. Our simple estimates show that the improvement in the solid–liquid electrolyte interphase resistance observed here could translate to an enhancement of 15–22% in the practical energy density of a Li–S or Li–O2 battery and improvements in the roundtrip efficiency of 21–28 percentage points.

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Accepted/In Press date: 29 November 2021
e-pub ahead of print date: 28 December 2021
Keywords: electrolyte additives, lithium metal batteries, lithium-ion transport, solid-liquid electrolyte interphases, solid-liquid hybrid electrolytes

Identifiers

Local EPrints ID: 452870
URI: http://eprints.soton.ac.uk/id/eprint/452870
ISSN: 1944-8244
PURE UUID: fe8cc033-8921-4a51-9a0c-de1d74118a20
ORCID for Nuria Garcia-Araez: ORCID iD orcid.org/0000-0001-9095-2379
ORCID for Vivek Padmanabhan: ORCID iD orcid.org/0000-0002-6088-312X
ORCID for Nina Meddings: ORCID iD orcid.org/0000-0001-7242-6076

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Date deposited: 06 Jan 2022 17:37
Last modified: 28 Apr 2022 02:18

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Contributors

Author: Vivek Padmanabhan ORCID iD
Author: Nina Meddings ORCID iD

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