Ordered Co‐Assembly of Soft‐in‐Hard Hetero‐Structured Pulse Guidance Ion‐Accelerator for Dendrite‐Free Aqueous Zinc‐Ion Battery Anodes

Constructing a solid electrolyte interface (SEI) layer to suppress dendrite growth is an effective approach in Zn-based aqueous batteries. Traditional SEI layers are limited by their simple structure and composition, enabling only one functionality of either providing nucleation sites or facilitating desolvation. In this study, a pulse guidance ion-accelerator is constructed by kinetics-controlled co-assembly of zincophilic micelles and zincophobic metal-organic framework (MOF). The closely packed soft micelles, in conjunction with the hard MOF host particles, form a multi-tiered soft-in-hard hetero-structure that accelerates adsorption, pre-desolvation, and subsequent desolvation processes, facilitating the (002) crystal plane dendrite-free deposition. As a result, stable cycling over 1900 h (31 mV polarization) in symmetric cell and 5200 cycles in the Zn//Cu battery (99.8% coulombic efficiency) can be achieved. These findings will effectively promote the development of stable and long-cycling aqueous zinc-ion batteries.