Intrinsic Interfacial Dynamic Engineering of Zincophilic Microbrushes via Regulating Zn Deposition for Highly Reversible Aqueous Zinc Ion Battery

Abstract Aqueous rechargeable zinc ion batteries are promising efficient energy storage systems due to remarkable safety and satisfactory capacity. However, zinc metal anode instability including dendrite growth and side reactions severely hinders widespread applications. Herein, zincophilic microbrushes have been in situ anchored on zinc plates through simple freeze‐drying and mild reduction of graphene oxide, successfully overcoming these thorny issues. By introducing suitable oxygen‐containing groups, the microbrushes exhibit a good affinity for zinc ions, thereby providing sufficient depositing sites, promoting zinc plating and stripping during cycling, and suppressing side reactions. The delicate zincophilic microbrushes can not only function as protective layer to guide the deposition of zinc ions, but also act as high‐speed pathways to redistribute the zinc ion flux for rapid kinetics. Consequently, the microbrushes‐covered zinc anode displays long lifespan and good durability, whenever in symmetric cell or full battery tests. This work paves a feasible bridge to design advanced aqueous anodes by architecting both structures and compositions of metal coverings.