Understanding Thermodynamic and Kinetic Contributions in Expanding the Stability Window of Aqueous Electrolytes

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Jiaxin Zheng
  • Guoyu Tan
  • Peng Shan
  • Tongchao Liu
  • Jiangtao Hu
  • Yancong Feng
  • Luyi Yang
  • Mingjian Zhang
  • Zonghai Chen
  • Yuan Lin
  • Jun Lu
  • Joerg C. Neuefeind
  • Khalil Amine
  • Lin-Wang Wang
  • Kang Xu
  • Feng Pan

Detail(s)

Original languageEnglish
Pages (from-to)2872-2882
Journal / PublicationChem
Volume4
Issue number12
Publication statusPublished - 13 Dec 2018
Externally publishedYes

Abstract

Because of their non-flammable nature, low toxicity, and low production cost, aqueous Li-ion batteries (LIBs) promise very tempting alternatives to the state-of-the-art LIBs that rely on highly flammable and toxic non-aqueous electrolytes. However, the intrinsic narrow electrochemical stability window (1.23 V) of water sets an upper limit on the practical voltage and energy output. Here, we report a super-concentrated (unsaturated) LiNO3-based aqueous electrolyte that effectively expands the aqueous stability window to 2.55 V. We further revealed that a unique local structure with (Li+(H2O)2)n polymer-like aggregation arises at the super-concentration, which assists in stabilizing the aqueous solution at extreme potentials via both thermodynamic and kinetic contributions. This fundamental revelation of liquid structure and its effect on the electrochemical stability window provides a new pathway for designing high-voltage aqueous electrolytes.

Research Area(s)

  • aqueous electrolyte, electrochemical stability window, LiNO3 aqueous solution, molecular dynamics simulation, pair-distribution function, polymer-like chains, SDG7: Affordable and clean energy, super-concentrated

Bibliographic Note

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Citation Format(s)

Understanding Thermodynamic and Kinetic Contributions in Expanding the Stability Window of Aqueous Electrolytes. / Zheng, Jiaxin; Tan, Guoyu; Shan, Peng; Liu, Tongchao; Hu, Jiangtao; Feng, Yancong; Yang, Luyi; Zhang, Mingjian; Chen, Zonghai; Lin, Yuan; Lu, Jun; Neuefeind, Joerg C.; Ren, Yang; Amine, Khalil; Wang, Lin-Wang; Xu, Kang; Pan, Feng.

In: Chem, Vol. 4, No. 12, 13.12.2018, p. 2872-2882.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review