Self-assembled Tetrabutanol nanoclusters for interfacial regulation of zinc anodes enabling high-stability aqueous zinc-ion batteries.

The water-induced parasitic reactions and uncontrolled dendritic growth at the zinc anode/electrolyte interface significantly hinder the practical application of aqueous zinc-ion batteries (AZIBs) in large-scale energy storage. Herein, we propose a novel strategy to optimize the electrode-electrolyte system through the in situ self-assembly of tetrabutanol clusters derived from the hydrolysis of tetrabutyl titanate (TBT). This approach reconstructs the hydrogen-bonding network of the electrolyte, effectively suppressing the activity of water species. Meanwhile, an organic-inorganic hybrid dual-layer interface enriched with tetrabutanol nanoclusters and ZnCO3/ZnS compounds are constructed at the Zn anode-electrolyte interface. This approach is beneficial for the desolvation of zinc ions and the nucleation kinetics of Zn2+, inhibits the hydrogen evolution reaction (HER), and induces the uniform deposition of Zn2+ on the (002) crystal plane of the zinc anode. Consequently, the Zn||Zn symmetric cell with TBT additive achieves exceptional cycling stability exceeding 1600 h at 2 mA cm-2 and 1 mAh cm-2. The Zn||Cu asymmetric cell exhibits an average Coulombic efficiency of 99.7 % over 1300 cycles. Furthermore, the Zn||NH4V4O10 full cell presents a high capacity retention rate after 1000 cycles. This study provides a new interfacial regulation strategy for the development of high-performance aqueous zinc-ion batteries.