High entropy electrolyte modifies electrode/electrolyte interface promoting highly reversible zinc anode

Aqueous zinc-ion batteries (AZIBs) have drawn considerable interest owing to their affordability, safety, and eco-friendly nature. Unfortunately, the uneven deposition on the Zn anode promotes the growth of dendrites, and the corrosion of Zn by interfacial active water triggers a severe hydrogen evolution reaction (HER), which greatly hampers the further application of AZIBs. Therefore, a high-entropy (HE) electrolyte strategy is proposed to achieve a highly reversible Zn metal anode and an improved electrode/electrolyte interface (EEI). Specifically, this HE electrolyte achieves a water-poor solvation structure through N'N dimethylformamide (DMF) modulation of the solvation structure and accelerates Zn 2+ diffusion. The dynamic adsorption processes of benzylideneacetone (BDA) and DMF adsorption on the Zn anode strengthen the electrode-electrolyte interface, promoting uniform Zn deposition and interfacial stability are achieved. Consequently, Zn||Zn symmetric cells demonstrate cycle stability exceeding 1400 h, while Zn||Cu cells achieve an average Coulombic efficiency of 99.63% over 750 cycles. In addition, full cells assembled with this electrolyte demonstrates their great potential for practical applications. This study provides a promising idea for designing high-performance aqueous high-entropy electrolytes. Aqueous zinc-ion batteries suffer from dendrite growth, byproduct accumulation, and freezing at low temperatures. We successfully suppressed dendrite growth and side reactions by introducing multiple compounds into the electrolyte to increase its disorder and construct a high-entropy electrolyte. This disrupted the original hydrogen-bond network in the electrolyte and enhanced the battery's cycling performance at low temperatures. • A high-entropy electrolyte has been successfully developed, and its melting point has been reduced. • The addition of multiple components disrupts the original hydrogen-bond network in the electrolyte, altering the solvation structure of Zn 2+ . • This electrolyte significantly enhances the reversibility of Zn deposition/stripping, with the Zn anode exhibiting a smooth planar surface after cycling.