Bioinspired Repurposing of Lisinopril: A Clinical ACE Inhibitor as a Trace Dual‐Functional Additive for Ultrastable Aqueous Zinc‐Ion Batteries

ABSTRACT

The practical deployment of aqueous zinc‐ion batteries (AZIBs) is critically hindered by rampant dendrite growth and parasitic side reactions, originating from unregulated Zn ^{2 +} solvation chemistry and unstable electrode‐electrolyte interfaces. Inspired by the zinc‐targeting molecular recognition mechanism of angiotensin‐converting‐enzyme (ACE) inhibitors, we repurpose clinical drug lisinopril (LIS) as a trace multifunctional electrolyte additive for high‐performance AZIBs. The multidentate and amphiphilic structure of LIS orchestrates a synergistic dual‐regulation mechanism: LIS spontaneously adsorbs and in situ assembles into a robust gradient organic–inorganic hybrid solid electrolyte interphase that homogenizes Zn ²⁺ flux and establishes a water‐depleted electric double layer by its hydrophobic moieties; meanwhile LIS alters the [Zn(H ₂ O) ₆ ] ²⁺ solvation shell, disrupts the native hydrogen‐bond network, and buffers interfacial pH fluctuations at the anode interface. Consequently, trace LIS enables highly reversible Zn plating/stripping, with Zn||Cu cells delivering an average Coulombic efficiency of 99.78% over 1500 cycles and Zn||Zn cells operating for 2400 h at 4 mA cm ⁻² /4 mAh cm ⁻² . Remarkably, the LIS‐containing full cells retain 77.25% of their capacity after 10 000 cycles, and pouch cells maintain 74.46% capacity after 600 cycles. This work illustrates that pharmaceutical molecules with inherent Zn‐binding motifs can be converted into function‐oriented electrolyte additives to achieve durable AZIBs.