Unlocking Anode-Free Zinc Metal Batteries via Data-Science-Guided Dual-Interphase Separator Engineering

Aqueous zinc metal batteries (AZMBs) employing halogen- or manganese-based cathodes and anode-free design possess the highest energy density among the aqueous battery families. However, their performance is severely limited by interfacial side reactions and anode-cathode cross-talk, which undermine energy density and cycle life. Conventional strategies focusing on a single interface are inadequate to address these systemic issues. The optimal strategy cluster from literature data mining guided the material system creation via a data-driven process of molecular descriptor screening. This guided the creation of an asymmetric dual-interphase separator, featuring a Zn²⁺-supplying interphase (ZSI) on the anode side that suppresses polyhalide shuttling and accelerates desolvation, and a composite conductive interphase (CCI) on the cathode side that enhances multi-electron reaction kinetics and active species utilization. Enabled by the asymmetric dual-interphase engineering, the constructed anode-free Zn||MnO₂ full cell achieves a high voltage efficiency of 90% and stable cycling over 1000 cycles. Concurrently, a state-of-the-art anode-free Zn||I₂ battery delivers an energy efficiency exceeding 90% at high areal loading of 38.14 mg cm^-2. Furthermore, a universal zinc metal anode/electrolyte interphase descriptor (ZMAEID) was proposed, mechanistically linking interfacial electrochemical behavior with mechanical stability. This systematic, data-driven, and theory-guided strategy establishes a new paradigm for next-generation anode-free AZMBs.