Gel Electrolyte Interdigitation Enables Stable High Areal Capacity Cycling of the 3D Zn Electrode

Abstract

Inferior rechargeability of the metallic zinc anode, especially under high areal capacities and moderate to high current densities, remains a significant bottleneck for developing scalable aqueous zinc-ion batteries. While three-dimensional (3D) porous zinc anodes can mitigate high local current density and enhance deposition kinetics, limited electrolyte percolation within the 3D framework with conventional liquid electrolyte-soaked separator leads to surface-concentrated ion flux, which confines zinc nucleation and growth to the uppermost surface. This results in early short-circuit events mediated by dendrites. Here, electrolyte-interdigitation with a biopolymer hydrogel electrolyte is presented as a facile strategy, which by design enables complete electrolyte percolation within the porous and tortuous structure of the 3D zinc and uniform mass transport across the whole electrode structure. The increased accessible surface area and interconnected transport pathways effectively regulate zinc plating/stripping, thus maintaining the structural integrity upon cycling. As a result, the integrated design enables extended zinc rechargeability and a cumulative cycling capacity of 1680 mAh cm−2 under demanding 5 mA cm⁻² - 5 mAh cm⁻² conditions. Suppressed corrosion and dendrite inhibition for the interdigitated anode also lead to excellent rate capability and stability of the full-cell, highlighting a significant advance in the field of 3D zinc anode design.

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Article information

Article type
Paper
Submitted
19 Dec 2024
Accepted
25 Feb 2025
First published
27 Feb 2025
This article is Open Access
Creative Commons BY license

J. Mater. Chem. A, 2025, Accepted Manuscript

Gel Electrolyte Interdigitation Enables Stable High Areal Capacity Cycling of the 3D Zn Electrode

Y. Shang, R. Kokate, P. Tung, H. Zhong, E. Lizundia, F. J. Trujillo, P. V. Kumar and D. Kundu, J. Mater. Chem. A, 2025, Accepted Manuscript , DOI: 10.1039/D4TA09006C

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