Wood-inspired anisotropic hydrogel electrolyte with large modulus and low tortuosity realizing durable dendrite-free zinc-ion batteries

Author:

Chen Jizhang1ORCID,Chen Minfeng1ORCID,Chen Hongli2ORCID,Yang Ming3,Han Xiang1ORCID,Ma Dingtao3,Zhang Peixin3,Wong Ching-Ping4

Affiliation:

1. Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China

2. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

3. College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China

4. School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA 30332

Abstract

While aqueous zinc-ion batteries exhibit great potential, their performance is impeded by zinc dendrites. Existing literature has proposed the use of hydrogel electrolytes to ameliorate this issue. Nevertheless, the mechanical attributes of hydrogel electrolytes, particularly their modulus, are suboptimal, primarily ascribed to the substantial water content. This drawback would severely restrict the dendrite-inhibiting efficacy, especially under large mass loadings of active materials. Inspired by the structural characteristics of wood, this study endeavors to fabricate the anisotropic carboxymethyl cellulose hydrogel electrolyte through directional freezing, salting-out effect, and compression reinforcement, aiming to maximize the modulus along the direction perpendicular to the electrode surface. The heightened modulus concurrently serves to suppress the vertical deposition of the intermediate product at the cathode. Meanwhile, the oriented channels with low tortuosity enabled by the anisotropic structure are beneficial to the ionic transport between the anode and cathode. Comparative analysis with an isotropic hydrogel sample reveals a marked enhancement in both modulus and ionic conductivity in the anisotropic hydrogel. This enhancement contributes to significantly improved zinc stripping/plating reversibility and mitigated electrochemical polarization. Additionally, a durable quasi-solid-state Zn//MnO 2 battery with noteworthy volumetric energy density is realized. This study offers unique perspectives for designing hydrogel electrolytes and augmenting battery performance.

Funder

JST | Natural Science Foundation of Jiangsu Province

MOST | National Natural Science Foundation of China

Publisher

Proceedings of the National Academy of Sciences

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