The synergistic effect induced by "Z-bond" between cations and anions achieving a highly reversible zinc anode

J Colloid Interface Sci. 2024 Dec 20;683(Pt 2):92-105. doi: 10.1016/j.jcis.2024.12.129. Online ahead of print.

Abstract

Due to their high energy density, low cost, and environmental friendliness, aqueous zinc-ion batteries are considered a potential alternative to Li-ion batteries. However, dendrite growth and parasitic reactions of water molecules limit their practical applications. Herein, an ionic liquid additive, 1-butyl-3-methylimidazolium Bis(fluorosulfonyl)imide (BMImFSI), is introduced to regulate the electrical double layer (EDL). Both BMIm+ and FSI- can preferentially adsorb on the Zn anode, constructing a water-poor EDL and thus effectively suppressing side reactions. Additionally, under the synergistic effect of the mineralized solid-electrolyte interphase (SEI) formed by the decomposition of FSI- and the ion dispersion layer constructed by BMIm+ on the mineralized SEI, the deposition of zinc ions is effectively dispersed, preventing excessive aggregation of zinc ions and thus dendrite formation. The Zn‖Zn symmetric cells using the BMImFSI/ZnSO4 electrolyte operate stably for 1060 h and 560 h at 10 mA cm-2-10 mAh cm-2 and 20 mA cm-2-20 mAh cm-2, respectively. The Zn‖Cu asymmetric cell maintains an average Coulombic efficiency of 99.4 % after 1000 cycles. The capacity retention of a full cell using α-MnO2 as the cathode is significantly improved at 1 A g-1.

Keywords: Aqueous zinc-ion battery; BMImFSI additive; Solid electrolyte interphase; Synergistic effect; Z-bond.