An Organic‐Inorganic‐Integrated Solid Electrolyte Interphase with High‐Resilience and Anti‐Corrosion for Sustainable Zinc Metal Anode

Abstract Aqueous zinc metal batteries (AZMBs) are highly regarded for their exceptional safety, low cost, environmental compatibility, and potential as a sustainable alternative to lithium‐ion batteries. However, Zn dendrite growth and hydrogen evolution on anode side result in limited lifespan and safety issues. Herein, an organic‐inorganic‐integrated solid electrolyte interphase (SEI) was in situ formed by adding 4‐(trifluoromethyl)‐1H‐imidazole (TFMI) as an electrolyte additive. The artificial SEI merited higher maximum elastic deformation energy due to relatively high resilience and toughness, which can prevent Zn dendrite penetration and anode self‐cracking and pulverization. In addition, N‐containing heterocycles in SEI act as a H + catcher, thereby inhibiting anode corrosion and hydrogen evolution. As a result, the Zn||Zn symmetric cell has delivered stable cycling performance after 1500 h at 5 mA cm −2 with a terminated capacity of 5 mAh cm −2 . And an outstanding coulombic efficiency of 99.46% at the 2200th cycle was achieved for a Cu||Zn asymmetric cell. Furthermore, a Zn||PANI full battery presented a stable cycling performance with a high‐capacity retention of 97.6% after 200 cycles.