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

Abstract 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.