Two Birds with One Stone: Green Solvent Enabled High‐Stability and Durable Zn Anode in Both Non‐Aqueous and Aqueous Electrolytes

Abstract Rechargeable zinc batteries are promising choices for eco‐friendly, safe and cost‐effective energy storage solutions. However, their commercial adoption faces challenges such as low Coulombic efficiency (CE) and poor reversibility of Zn anodes. To address these issues, a new green electrolyte based on N,N'‐Dimethylpropyleneurea (DMPU) has been developed, affording a robust, dendrite‐free Zn anode with over 5000 h of cycle stability and a high average CE of 98.49%. Zn anode in DMPU‐electrolyte significantly outperforms aqueous electrolyte with 67 times longer cycle life, demonstrating excellent anode stability. Moreover, ultra‐stable Zn anode in DMPU‐electrolyte cycled for over 10 000 cycles at 1.0 mA cm⁻² showcases excellent reversibility. The Dimethylpropyleneurea‐triflate anion generated solid electrolyte interphase enables homogeneous and rapid Zn²⁺‐diffusion at the electrode interface, leading to a structured hexagonal Zn deposit. Furthermore, as electrolyte additive, DMPU significantly stabilizes Zn anode at severe conditions (5.0 and 10.0 mA cm⁻²) along with remarkable enhancement in CE (99.12%). This study offers valuable insights into the development of hybrid and organic electrolytes to advance Zn battery technology.