Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating

Chang Li; Ryan Kingsbury; Laidong Zhou; Abhinandan Shyamsunder; Kristin A. Persson; Linda F. Nazar

doi:10.1021/acsenergylett.1c02514

Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating

Chang Li, Ryan Kingsbury, Laidong Zhou, Abhinandan Shyamsunder, Kristin A. Persson, Linda F. Nazar

Research output: Contribution to journal › Article › peer-review

93 Scopus citations

Abstract

Aqueous zinc batteries are recognized to suffer from H⁺/Zn²⁺ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H⁺ intercalation. Herein, we realize this goal by tuning the solvation structure, using LiV₂(PO₄)₃ (LVP) as a model cathode. Phase conversion of LVP induced by H⁺ intercalation is observed in 4 m Zn(OTf)₂, whereas dominant Zn²⁺ insertion is confirmed in a ZnCl₂ water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn²⁺–H₂O interaction in the latter that interrupts the H₂O hydrogen bonding network, thus suppressing H⁺ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl₂ WiSE. This system exhibits an optimized Zn²⁺ solvation sheath with a similar low free water content, showing not only much better suppression of H⁺ intercalation but also highly reversible Zn plating/stripping with a CE of ∼99.7% over 150 cycles.

Original language	English (US)
Pages (from-to)	533-540
Number of pages	8
Journal	ACS Energy Letters
Volume	7
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.1c02514
State	Published - Jan 14 2022
Externally published	Yes

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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title = "Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating",

abstract = "Aqueous zinc batteries are recognized to suffer from H+/Zn2+ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H+ intercalation. Herein, we realize this goal by tuning the solvation structure, using LiV2(PO4)3 (LVP) as a model cathode. Phase conversion of LVP induced by H+ intercalation is observed in 4 m Zn(OTf)2, whereas dominant Zn2+ insertion is confirmed in a ZnCl2 water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn2+–H2O interaction in the latter that interrupts the H2O hydrogen bonding network, thus suppressing H+ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl2 WiSE. This system exhibits an optimized Zn2+ solvation sheath with a similar low free water content, showing not only much better suppression of H+ intercalation but also highly reversible Zn plating/stripping with a CE of ∼99.7% over 150 cycles.",

author = "Chang Li and Ryan Kingsbury and Laidong Zhou and Abhinandan Shyamsunder and Persson, {Kristin A.} and Nazar, {Linda F.}",

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AU - Li, Chang

AU - Kingsbury, Ryan

AU - Zhou, Laidong

AU - Shyamsunder, Abhinandan

AU - Persson, Kristin A.

AU - Nazar, Linda F.

PY - 2022/1/14

Y1 - 2022/1/14

N2 - Aqueous zinc batteries are recognized to suffer from H+/Zn2+ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H+ intercalation. Herein, we realize this goal by tuning the solvation structure, using LiV2(PO4)3 (LVP) as a model cathode. Phase conversion of LVP induced by H+ intercalation is observed in 4 m Zn(OTf)2, whereas dominant Zn2+ insertion is confirmed in a ZnCl2 water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn2+–H2O interaction in the latter that interrupts the H2O hydrogen bonding network, thus suppressing H+ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl2 WiSE. This system exhibits an optimized Zn2+ solvation sheath with a similar low free water content, showing not only much better suppression of H+ intercalation but also highly reversible Zn plating/stripping with a CE of ∼99.7% over 150 cycles.

AB - Aqueous zinc batteries are recognized to suffer from H+/Zn2+ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H+ intercalation. Herein, we realize this goal by tuning the solvation structure, using LiV2(PO4)3 (LVP) as a model cathode. Phase conversion of LVP induced by H+ intercalation is observed in 4 m Zn(OTf)2, whereas dominant Zn2+ insertion is confirmed in a ZnCl2 water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn2+–H2O interaction in the latter that interrupts the H2O hydrogen bonding network, thus suppressing H+ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl2 WiSE. This system exhibits an optimized Zn2+ solvation sheath with a similar low free water content, showing not only much better suppression of H+ intercalation but also highly reversible Zn plating/stripping with a CE of ∼99.7% over 150 cycles.

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Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating

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