Aqueous zinc‐ion batteries (AZIBs) are widely recognized as a promising candidate for energy storage owing to their intrinsic safety, environmental benignity, and low cost. Nevertheless, the unstable Zn/electrolyte interphase leads to uncontrolled dendritic growth, parasitic side reactions, and the accumulation of insulating byproducts, all of which hinder their practical deployment. Herein, we introduce a trace amount (0.5 vol%) of N‐methylpyrrolidone as an efficient electrolyte additive to in situ construct an inorganic‐rich solid electrolyte interphase (SEI) in a dilute ZnSO 4 electrolyte. The compact and uniform SEI layer on the Zn anode surface takes a role as a protective barrier that prevents direct contact between the electrode and the electrolyte, thereby suppressing corrosion and other parasitic reactions. As a result, the Zn||Zn symmetric cell exhibits highly reversible plating/stripping for over 200 h under a high areal capacity of 8 mAh cm −2 (depth of discharge ~ 68.3%). This article provides a practical and scalable strategy for interfacial regulation in aqueous Zn systems and offers valuable insights into the rational design of electrolyte additives for high‐performance AZIBs.
Xiao et al. (Fri,) studied this question.