ABSTRACT Aqueous zinc metal batteries (AZMBs) have attracted considerable attention due to their inherent safety and low cost. However, their development has been significantly impeded by the sluggish Zn 2+ transport and instable aqueous interface. Here, we introduce basic amino acids as multifunctional electrolyte additives to tackle this issue, with L‐arginine (Arg) selected as a representative case for in‐depth mechanistic investigation. We elucidate that protonated Arg (Arg + ) restricts SO 4 2− anions migration by forming large‐size anion clusters via electrostatic interactions. Concurrently, it constructs a hydrophobic, O‐down oriented, and low‐reactivity water microenvironment at the electrode‐electrolyte interface. This coordinated regulation of the bulk electrolyte and the electrode‐electrolyte interface optimizes Zn 2+ migration kinetics and reduction thermodynamics, effectively suppressing side reactions and eliminating disordered dendrite growth. Consequently, the zinc anode achieves highly reversible stripping/plating efficiency of 99.43% at 0.5 mA cm −2 and 0.5 mAh cm −2 , and demonstrates stable cycling for over 1200 h at 5 mA cm −2 and 5 mAh cm −2 . Furthermore, Zn//VOX full coin cells retain 74.5% capacity after 1200 cycles at 2 A g −1 , and 2.28 Ah‐level pouch cell maintains 80.5% capacity after 160 cycles. This work establishes a multiscale framework for additive‐electrolyte interactions and provides a molecular design strategy for aqueous battery additives.
Tao et al. (2026) studied this question.