Tuning Zn Ion Diffusion and Desolvation Via Zincophilic Carbonyl-Rich Interphase Towards Highly Reversible and Dendrite-Free Zinc Anodes

Abstract

Serious dendrite formation and sluggish dynamics at Zn anode hinder the commercialization of aqueous zinc-ion batteries (AZIBs). Here, a zincophilic and carbonyl-rich zinc citrate interphase was in-situ constructed on Zn anode surface (Zn@CZ) to overcome the above-mentioned challenges. Finding confirms that the introduced zinc citrate layer could effectively homogenize the interfacial electric field distribution and favor Zn2+ transport at the anode due to the reduced nucleation barrier. Moreover, the functional oxygen-containing groups on Zn@CZ electrode accelerate the Zn2+ desolvation process and isolate the electrolytes, which further restrains the water-related parasitic reactions. As a result, the Zn@CZ anode exhibits an ultralong cycle lifespan of 6270 h at 1 mA cm-2/0.5 mAh cm-2, and maintains long-term stability for 4320 h at 5 mA cm−2/2 mAh cm-2 with a high cumulative plated capacity (10.8 Ah cm-2). The Zn@CZ//MnO2 full cells also achieve an excellent retention rate of 88.2% after 1100 cycles. The work brings forward a facile and industry-compatible approach towards dendrite-free and high reversible AZIBs.

Keywords: Zinc anode, Carbonyl-rich interphase, Dendrite-free, Zincophilicity, Interfacial modification