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Interfacial Chemistry in Aqueous Lithium-Ion Batteries : A Case Study of V2O5 in Dilute Aqueous Electrolytes

Hou, Xu LU orcid ; Zhang, Leiting ; Gogoi, Neeha ; Edström, Kristina and Berg, Erik J. (2024) In Small 20(23).
Abstract

Aqueous lithium-ion batteries (ALIBs) are promising for large-scale energy storage systems because of the cost-effective, intrinsically safe, and environmentally friendly properties of aqueous electrolytes. Practical application is however impeded by interfacial side-reactions and the narrow electrochemical stability window (ESW) of aqueous electrolytes. Even though higher electrolyte salt concentrations (e.g., water-in-salt electrolyte) enhance performance by widening the ESW, the nature and extent of side-reaction processes are debated and more fundamental understanding thereof is needed. Herein, the interfacial chemistry of one of the most popular electrode materials, V2O5, for aqueous batteries is... (More)

Aqueous lithium-ion batteries (ALIBs) are promising for large-scale energy storage systems because of the cost-effective, intrinsically safe, and environmentally friendly properties of aqueous electrolytes. Practical application is however impeded by interfacial side-reactions and the narrow electrochemical stability window (ESW) of aqueous electrolytes. Even though higher electrolyte salt concentrations (e.g., water-in-salt electrolyte) enhance performance by widening the ESW, the nature and extent of side-reaction processes are debated and more fundamental understanding thereof is needed. Herein, the interfacial chemistry of one of the most popular electrode materials, V2O5, for aqueous batteries is systematically explored by a unique set of operando analytical techniques. By monitoring electrode/electrolyte interphase deposition, electrolyte pH, and gas evolution, the highly dynamic formation/dissolution of V2O5/V2O4, Li2CO3 and LiF during dis-/charge is demonstrated and shown to be coupled with electrolyte decomposition and conductive carbon oxidation, regardless of electrolyte salt concentration. The study provides deeper understanding of interfacial chemistry of active materials under variable proton activity in aqueous electrolytes, hence guiding the design of more effective electrode/electrolyte interfaces for ALIBs and beyond.

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author
; ; ; and
publishing date
type
Contribution to journal
publication status
published
keywords
dilute aqueous electrolytes, electrode/electrolyte interphase, operando characterization, VO
in
Small
volume
20
issue
23
article number
2308577
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85180523948
  • pmid:38145960
ISSN
1613-6810
DOI
10.1002/smll.202308577
language
English
LU publication?
no
additional info
Publisher Copyright: © 2023 The Authors. Small published by Wiley-VCH GmbH.
id
33ce0c78-a770-4908-a76b-48b4f98eef1e
date added to LUP
2025-12-05 22:22:58
date last changed
2026-01-31 03:41:35
@article{33ce0c78-a770-4908-a76b-48b4f98eef1e,
  abstract     = {{<p>Aqueous lithium-ion batteries (ALIBs) are promising for large-scale energy storage systems because of the cost-effective, intrinsically safe, and environmentally friendly properties of aqueous electrolytes. Practical application is however impeded by interfacial side-reactions and the narrow electrochemical stability window (ESW) of aqueous electrolytes. Even though higher electrolyte salt concentrations (e.g., water-in-salt electrolyte) enhance performance by widening the ESW, the nature and extent of side-reaction processes are debated and more fundamental understanding thereof is needed. Herein, the interfacial chemistry of one of the most popular electrode materials, V<sub>2</sub>O<sub>5</sub>, for aqueous batteries is systematically explored by a unique set of operando analytical techniques. By monitoring electrode/electrolyte interphase deposition, electrolyte pH, and gas evolution, the highly dynamic formation/dissolution of V<sub>2</sub>O<sub>5</sub>/V<sub>2</sub>O<sub>4</sub>, Li<sub>2</sub>CO<sub>3</sub> and LiF during dis-/charge is demonstrated and shown to be coupled with electrolyte decomposition and conductive carbon oxidation, regardless of electrolyte salt concentration. The study provides deeper understanding of interfacial chemistry of active materials under variable proton activity in aqueous electrolytes, hence guiding the design of more effective electrode/electrolyte interfaces for ALIBs and beyond.</p>}},
  author       = {{Hou, Xu and Zhang, Leiting and Gogoi, Neeha and Edström, Kristina and Berg, Erik J.}},
  issn         = {{1613-6810}},
  keywords     = {{dilute aqueous electrolytes; electrode/electrolyte interphase; operando characterization; VO}},
  language     = {{eng}},
  month        = {{06}},
  number       = {{23}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Small}},
  title        = {{Interfacial Chemistry in Aqueous Lithium-Ion Batteries : A Case Study of V<sub>2</sub>O<sub>5</sub> in Dilute Aqueous Electrolytes}},
  url          = {{http://dx.doi.org/10.1002/smll.202308577}},
  doi          = {{10.1002/smll.202308577}},
  volume       = {{20}},
  year         = {{2024}},
}