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2D Mesoporous Polydopamine Nanosheets Break the Strength–Conductivity Trade-Off in Hydrogel Electrolytes Toward Stable Zn Anodes
DOI:10.1002/adfm.76140.png)
Abstract
En 中文
Hydrogel electrolytes are attractive for aqueous zinc-ion batteries, but simultaneously achieving mechanical robustness, fast Zn2+ transport, and interfacial stability remains challenging. Herein, we show that two-dimensional mesoporous polydopamine nanosheets (2D-mPDA) act as multifunctional polymeric nanofillers in a poly(vinyl alcohol)-based hydrogel electrolyte for stabilizing Zn anodes. The polymer-compatible 2D framework, in-plane mesoporous ion-transport channels, and catechol/amine-rich surface chemistry endow the electrolyte with an ionic conductivity of 31.36 mS cm−1, a tensile strength of 1.52 MPa, and a Zn2+ transference number of 0.79, thereby overcoming the usual trade-off between mechanical strength and ionic conductivity. Experiments and simulations reveal that 2D-mPDA reconstructs the hydrogen-bonding network, suppresses water activity, and remodels the primary solvation shell of Zn2+ through catechol/amine coordination, which lowers the desolvation barrier, homogenizes Zn2+ flux, and enables dense Zn deposition. As a result, Zn||Zn symmetric cells cycle stably for over 7200 h at 1 mA cm−2, while Zn||VO2 full cells retain 90.2% of their capacity after 1500 cycles at 1 A g−1 and remain operational under severe deformation. This work highlights the importance of nanofiller design in hydrogel electrolytes for stabilizing Zn anodes and advancing durable aqueous zinc-ion batteries.
Keywords:
aqueous zinc-ion batteries
hydrogel electrolytes
mesoporous materials
polydopamine
two-dimensional materials
Journal
IF:
19
Papers:
3.4W
Citations:
32.1W

