Multiscale Computational Insights for Hydrogel Electrolytes in Aqueous Zinc Metal Batteries

ABSTRACT Aqueous zinc metal batteries (AZMBs) are promising due to their inherent safety, eco‐friendliness, and cost‐effectiveness. However, uncontrolled interfacial issues such as anode dendrites, hydrogen evolution, and cathode dissolution, adversely affect the cycling stability and capacity retention of AZMBs. Hydrogel electrolytes (HEs) could mitigate these issues but face practical limitations like mechanical fragility, interfacial instability, and temperature sensitivity. Furthermore, critical knowledge gaps persist in understanding cross‐scale structure‐property relationships from atomic‐scale to macroscale mechanical/electrochemical performance, and coupled mechanisms of charge/ion transfer and reaction kinetics in HEs. These gaps necessitate a multiscale computational perspective that bridge microscopic interactions and macroscopic functionality. Herein, we systematically discuss the challenges of HEs and the transformative role of multiscale computations in AZMBs. The intrinsic properties of HEs are first deconstructed through dual perspectives of electrochemical and physical characteristics, followed by critical challenges including the stability of the electrode/electrolyte interface. In response to these challenges, this review provides detailed insights of how multiscale computations, encompassing atomic/electronic, molecular, and macroscale approaches, elucidate the microscopic mechanisms of HE internal component interactions and electrolyte‐electrode interfacial behaviors at different scales. Finally, current challenges and prospects of multiscale computational frameworks for guiding the design of high‐performance HEs in AZMBs are discussed.