Built‐In Trimodal Molecular Interaction Effect Enables Interface‐Compatible and Temperature‐Tolerance Aqueous Zinc Batteries

Abstract Aqueous zinc‐ion batteries compatible with a wide temperature range and long cycle lifespan show great application prospects but are greatly limited by the unstable electrode‐electrolyte interfaces and mismatched electrolytes. This report presents the pathway of succinamic acid (SA) additive‐induced built‐in trimodal molecular interaction for constructing sustainable aqueous zinc batteries. As confirmed, such trimodal molecular interaction falls into the following patterns: the binding state of the H─F bond between SA and polyvinylidene fluoride (PVDF) binder, the micellar aggregation state in aqueous electrolyte, and the spontaneous adsorption state at Zn anode–electrolyte interface. Benefiting from the above synergistic effect, the Zn electrode shows a highly reversible deposition/stripping behavior over the wide temperature range (−10–50 °C) when paired with the optimized electrolyte. Specially, an impressive 3530 h‐cycle lifespan of the Zn symmetrical cell is achieved at the conditions of 1 mA cm −2 and 1 mAh cm −2 . Beyond that, significantly improved storage capability and cycle performance are demonstrated in both aqueous Zn‐MnO 2 and Zn‐I 2 batteries. Given the good balance between the working temperature range, ionic conductivity, and Zn 2+ transfer number of this trace molecule‐mediated electrolyte, this design paradigm provides new insights into developing advanced aqueous batteries, including but not limited to zinc‐based systems.