Regulating Surface Reaction Kinetics through Ligand Field Effects for Fast and Reversible Aqueous Zinc Batteries

Angew Chem Int Ed Engl. 2022 Nov 2;61(44):e202212780. doi: 10.1002/anie.202212780. Epub 2022 Sep 29.

Abstract

Designing water-deficient solvation sheath of Zn2+ by ligand substitution is a widely used strategy to protect Zn metal anode, yet the intrinsic tradeoff between Zn nucleation/dissolution kinetics and the side hydrogen evolution reaction (HER) remains a huge challenge. Herein, we find boric acid (BA) with moderate ligand field interaction can partially replace H2 O molecules in the solvation sheath of Zn2+ , forming a stable water-deficient solvation sheath. It enables fast Zn nucleation/dissolution kinetics and substantially suppressed HER. Crucially, by systematically comparing the ligand field strength and solvation energies between BA and the ever-reported electrolyte additives, we also find that the solvation energy has a strong correlation with Zn nucleation/dissolution kinetics and HER inhibition ability, displaying a classic volcano behavior. The modulation map could provide valuable insights for solvation sheath design of zinc batteries and beyond.

Keywords: Aqueous Zinc Batteries; Electrolyte Additive; Ligand Field Effects; Solvation Sheath; Surface Reaction Kinetics.