Intrinsic Ion ConcentrationDifference Induced AntipolyelectrolyteEffect for Promoting Stability of Zn Anodes

Aqueous zinc-ion batteries have gained significant attention due to their high safety and low cost. However, the cation concentration gradient at the anode/electrolyte interface often causes serious Zn dendrites and side reactions. Herein, cross-linked ion channels were constructed on the anode surface by the antipolyelectrolyte effect of zwitterionic polymer carboxymethyl chitosan (CMCHS) molecules, which is induced by the transient ion concentration difference at the initial Zn<sup>2+</sup> deposition process. The CMCHS channels endow the anode surface with homogeneous ions and electron distributions. Simultaneously, CMCHS molecules enter into Zn<sup>2+</sup> solvation structures and H<sub>2</sub>O molecules are removed, limiting the activity of solvated H<sub>2</sub>O molecules. Therefore, the dendrite growth and water activity are significantly suppressed, resulting in the excellent electrochemical performance of Zn anodes. An average Coulombic efficiency of 99.58% is achieved, which is much superior to the case in the conventional ZnSO<sub>4</sub> electrolyte. To illustrate the feasibility of the CMCHS-contained electrolyte, Zn||V<sub>2</sub>O<sub>5</sub> full batteries were assembled and exhibited enhanced electrochemical performance.

Publication Details

Journal
Figshare
Published
2025-03-10
DOI
https://doi.org/10.1021/jacs.4c15126.s001
Primary Topic
Advanced battery technologies research
Type
article
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article

Intrinsic Ion ConcentrationDifference Induced AntipolyelectrolyteEffect for Promoting Stability of Zn Anodes

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Advanced battery technologies research
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Intrinsic Ion ConcentrationDifference Induced AntipolyelectrolyteEffect for Promoting Stability of Zn Anodes

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Abstract

Aqueous zinc-ion batteries have gained significant attention due to their high safety and low cost. However, the cation concentration gradient at the anode/electrolyte interface often causes serious Zn dendrites and side reactions. Herein, cross-linked ion channels were constructed on the anode surface by the antipolyelectrolyte effect of zwitterionic polymer carboxymethyl chitosan (CMCHS) molecules, which is induced by the transient ion concentration difference at the initial Zn<sup>2+</sup> deposition process. The CMCHS channels endow the anode surface with homogeneous ions and electron distributions. Simultaneously, CMCHS molecules enter into Zn<sup>2+</sup> solvation structures and H<sub>2</sub>O molecules are removed, limiting the activity of solvated H<sub>2</sub>O molecules. Therefore, the dendrite growth and water activity are significantly suppressed, resulting in the excellent electrochemical performance of Zn anodes. An average Coulombic efficiency of 99.58% is achieved, which is much superior to the case in the conventional ZnSO<sub>4</sub> electrolyte. To illustrate the feasibility of the CMCHS-contained electrolyte, Zn||V<sub>2</sub>O<sub>5</sub> full batteries were assembled and exhibited enhanced electrochemical performance.

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Intrinsic Ion ConcentrationDifference Induced AntipolyelectrolyteEffect for Promoting Stability of Zn Anodes · Figshare (2025) | TGRS Research Map | TGRS