Biomimetic Superstructured Interphase for Aqueous Zinc-Ion Batteries
Yan Ai, Chaochao Yang, Ziqing Yin, Tong Wang, Tianyu Gai, Jiayou Feng, Kailin Li, Wei Zhang, Yefei Li, Fei Wang, Dongliang Chao, Yonggang Wang, Dongyuan Zhao, Wei Li
Abstract
The practical application of aqueous zinc-ion batteries (AZIBs) is greatly challenged by rampant dendrites and pestilent side reactions resulting from an unstable Zn–electrolyte interphase. Herein, we report the construction of a reliable superstructured solid electrolyte interphase for stable Zn anodes by using mesoporous polydopamine (2D-mPDA) platelets as building blocks. The interphase shows a biomimetic nacre’s “brick-and-mortar” structure and artificial transmembrane channels of hexagonally ordered mesopores in the plane, overcoming the mechanical robustness and ionic conductivity trade-off. Experimental results and simulations reveal that the −OH and −NH groups on the surface of artificial ion channels can promote rapid desolvation kinetics and serve as an ion sieve to homogenize the Zn 2+ flux, thus inhibiting side reactions and ensuring uniform Zn deposition without dendrites. The 2D-mPDA@Zn electrode achieves an ultralow nucleation potential of 35 mV and maintains a Coulombic efficiency of 99.8% over 1500 cycles at 5 mA cm –2 . Moreover, the symmetric battery exhibits a prolonged lifespan of over 580 h at a high current density of 20 mA cm –2 . This biomimetic superstructured interphase also demonstrates the high feasibility in Zn//VO 2 full cells and paves a new route for rechargeable aqueous metal-ion batteries.