Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries

Sailin Liu; Jianfeng Mao; Wei Kong Pang; Jitraporn Vongsvivut; Xiaohui Zeng; Lars Thomsen; Yanyan Wang; Jianwen Liu; Dan Li; Zaiping Guo

doi:10.1002/adfm.202104281

Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries

Sailin Liu, Jianfeng Mao^*, Wei Kong Pang, Jitraporn Vongsvivut, Xiaohui Zeng, Lars Thomsen, Yanyan Wang, Jianwen Liu, Dan Li, Zaiping Guo^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

403 Citations (Scopus)

Abstract

The cycle life of aqueous zinc-ion batteries (ZIBs) is limited by the notable challenges of cathode dissolution, water reactivity, and zinc dendrites. Here, it is demonstrated that by tuning the electrolyte solvation structure, the issues for both the electrodes and the electrolyte can be addressed simultaneously. Specifically, a fire-retardant triethyl phosphate (TEP) is demonstrated as a cosolvent with strong solvating ability in a nonaqueous/aqueous hybrid electrolyte. The TEP features a higher donor number (26 kcal mol⁻¹) than H₂O (18 kcal mol⁻¹), preferring to form a TEP occupied inner solvation sheath around Zn²⁺ and strong hydrogen bonding with H₂O. The TEP coordinated electrolyte structure can inhibit the reactivity of H₂O with V₂O₅ and leads to a robust polymeric-inorganic interphase (poly-ZnP₂O₆ and ZnF₂) on zinc anode effectively preventing the dendrite growth and parasitic water reaction. With such an optimized electrolyte, the Zn/Cu cells perform high average Coulombic efficiency of 99.5%, and the full cell with a low capacity ratio of Zn:V₂O₅ (2:1) and lean electrolyte (11.5 g Ah⁻¹) delivers a reversible capacity of 250 mAh g⁻¹ for over 1000 cycles at 5 A g⁻¹. This study highlights the promise of a successful electrolyte regulation strategy for the development of high-performance and practical ZIBs. © 2021 Wiley-VCH GmbH

Original language	English
Article number	2104281
Journal	Advanced Functional Materials
Volume	31
Issue number	38
Online published	3 Jul 2021
DOIs	https://doi.org/10.1002/adfm.202104281
Publication status	Published - 16 Sept 2021
Externally published	Yes

Funding

Financial support from the Australian Research Council (ARC) (LP160101629, LE180100141, DP210101486, and DP200101862) is acknowledged. S.L. would like to thank AINSE Limited for providing financial assistance (Award – PGRA). The contributions of the University of Wollongong (UOW) Electron Microscopy Centre by providing microscope facilities are gratefully acknowledged. The English editing of this manuscript by Dr. Tania Silver is also greatly appreciated.

Research Keywords

cathode dissolution
nonaqueous/aqueous hybrid electrolytes
triethyl phosphate
vanadium oxides
zinc-ion batteries

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries",

abstract = "The cycle life of aqueous zinc-ion batteries (ZIBs) is limited by the notable challenges of cathode dissolution, water reactivity, and zinc dendrites. Here, it is demonstrated that by tuning the electrolyte solvation structure, the issues for both the electrodes and the electrolyte can be addressed simultaneously. Specifically, a fire-retardant triethyl phosphate (TEP) is demonstrated as a cosolvent with strong solvating ability in a nonaqueous/aqueous hybrid electrolyte. The TEP features a higher donor number (26 kcal mol−1) than H2O (18 kcal mol−1), preferring to form a TEP occupied inner solvation sheath around Zn2+ and strong hydrogen bonding with H2O. The TEP coordinated electrolyte structure can inhibit the reactivity of H2O with V2O5 and leads to a robust polymeric-inorganic interphase (poly-ZnP2O6 and ZnF2) on zinc anode effectively preventing the dendrite growth and parasitic water reaction. With such an optimized electrolyte, the Zn/Cu cells perform high average Coulombic efficiency of 99.5%, and the full cell with a low capacity ratio of Zn:V2O5 (2:1) and lean electrolyte (11.5 g Ah−1) delivers a reversible capacity of 250 mAh g−1 for over 1000 cycles at 5 A g−1. This study highlights the promise of a successful electrolyte regulation strategy for the development of high-performance and practical ZIBs. {\textcopyright} 2021 Wiley-VCH GmbH",

keywords = "cathode dissolution, nonaqueous/aqueous hybrid electrolytes, triethyl phosphate, vanadium oxides, zinc-ion batteries",

author = "Sailin Liu and Jianfeng Mao and Pang, {Wei Kong} and Jitraporn Vongsvivut and Xiaohui Zeng and Lars Thomsen and Yanyan Wang and Jianwen Liu and Dan Li and Zaiping Guo",

year = "2021",

month = sep,

day = "16",

doi = "10.1002/adfm.202104281",

language = "English",

volume = "31",

journal = "Advanced Functional Materials",

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Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries. / Liu, Sailin; Mao, Jianfeng; Pang, Wei Kong et al.
In: Advanced Functional Materials, Vol. 31, No. 38, 2104281, 16.09.2021.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries

AU - Liu, Sailin

AU - Mao, Jianfeng

AU - Pang, Wei Kong

AU - Vongsvivut, Jitraporn

AU - Zeng, Xiaohui

AU - Thomsen, Lars

AU - Wang, Yanyan

AU - Liu, Jianwen

AU - Li, Dan

AU - Guo, Zaiping

PY - 2021/9/16

Y1 - 2021/9/16

N2 - The cycle life of aqueous zinc-ion batteries (ZIBs) is limited by the notable challenges of cathode dissolution, water reactivity, and zinc dendrites. Here, it is demonstrated that by tuning the electrolyte solvation structure, the issues for both the electrodes and the electrolyte can be addressed simultaneously. Specifically, a fire-retardant triethyl phosphate (TEP) is demonstrated as a cosolvent with strong solvating ability in a nonaqueous/aqueous hybrid electrolyte. The TEP features a higher donor number (26 kcal mol−1) than H2O (18 kcal mol−1), preferring to form a TEP occupied inner solvation sheath around Zn2+ and strong hydrogen bonding with H2O. The TEP coordinated electrolyte structure can inhibit the reactivity of H2O with V2O5 and leads to a robust polymeric-inorganic interphase (poly-ZnP2O6 and ZnF2) on zinc anode effectively preventing the dendrite growth and parasitic water reaction. With such an optimized electrolyte, the Zn/Cu cells perform high average Coulombic efficiency of 99.5%, and the full cell with a low capacity ratio of Zn:V2O5 (2:1) and lean electrolyte (11.5 g Ah−1) delivers a reversible capacity of 250 mAh g−1 for over 1000 cycles at 5 A g−1. This study highlights the promise of a successful electrolyte regulation strategy for the development of high-performance and practical ZIBs. © 2021 Wiley-VCH GmbH

AB - The cycle life of aqueous zinc-ion batteries (ZIBs) is limited by the notable challenges of cathode dissolution, water reactivity, and zinc dendrites. Here, it is demonstrated that by tuning the electrolyte solvation structure, the issues for both the electrodes and the electrolyte can be addressed simultaneously. Specifically, a fire-retardant triethyl phosphate (TEP) is demonstrated as a cosolvent with strong solvating ability in a nonaqueous/aqueous hybrid electrolyte. The TEP features a higher donor number (26 kcal mol−1) than H2O (18 kcal mol−1), preferring to form a TEP occupied inner solvation sheath around Zn2+ and strong hydrogen bonding with H2O. The TEP coordinated electrolyte structure can inhibit the reactivity of H2O with V2O5 and leads to a robust polymeric-inorganic interphase (poly-ZnP2O6 and ZnF2) on zinc anode effectively preventing the dendrite growth and parasitic water reaction. With such an optimized electrolyte, the Zn/Cu cells perform high average Coulombic efficiency of 99.5%, and the full cell with a low capacity ratio of Zn:V2O5 (2:1) and lean electrolyte (11.5 g Ah−1) delivers a reversible capacity of 250 mAh g−1 for over 1000 cycles at 5 A g−1. This study highlights the promise of a successful electrolyte regulation strategy for the development of high-performance and practical ZIBs. © 2021 Wiley-VCH GmbH

KW - cathode dissolution

KW - nonaqueous/aqueous hybrid electrolytes

KW - triethyl phosphate

KW - vanadium oxides

KW - zinc-ion batteries

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U2 - 10.1002/adfm.202104281

DO - 10.1002/adfm.202104281

M3 - RGC 21 - Publication in refereed journal

SN - 1616-301X

VL - 31

JO - Advanced Functional Materials

JF - Advanced Functional Materials

IS - 38

M1 - 2104281

ER -

Tuning the Electrolyte Solvation Structure to Suppress Cathode Dissolution, Water Reactivity, and Zn Dendrite Growth in Zinc-Ion Batteries

Abstract

Funding

Research Keywords

UN SDGs

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