Issue 30, 2024

Elucidating synergistic mechanisms of an anion–cation electrolyte additive for ultra-stable zinc metal anodes

Abstract

Uncontrollable dendrite formation and rampant parasitic reactions in zinc (Zn) metal anodes obstruct the practical application of aqueous Zn–metal batteries (AZMBs). Herein, we demonstrate a synergistic cation–anion regulation strategy to stabilize Zn metal anodes using NaI as a proof-of-concept additive for the ZnSO4 electrolyte system. By combining rigorous physicochemical, computational and electrochemical analyses, it is found that I anions can reshape the solvation sheath of Zn(H2O)62+, break the association of H2O and specifically absorb on the Zn surface, promoting Zn2+ transfer kinetics, guiding homogeneous Zn deposition and constraining parasitic reactions. Meanwhile, the Na+ cations absorb on irregular Zn tips as an electrostatic shielding to prevent dendrite growth. As a result, at an optimal additive concentration of 0.2 M, the Zn symmetric cells can deliver an astonishing 8632 h cyclability at 1 mA cm−2/1 mA h cm−2, exceeding by 83-fold that obtained using BE electrolyte. Furthermore, the additive supports highly reversible Zn stripping/plating at −10 °C, enables Zn‖NaV3O8·1.5H2O to attain significantly upgraded rate and cycling performances, and most importantly and uniquely, unlocks the high-capacity I/I3 redox couple for long-cycling Zn‖I batteries. This work provides a novel strategy to stabilize Zn metal anodes towards dendrite-free AZMBs.

Graphical abstract: Elucidating synergistic mechanisms of an anion–cation electrolyte additive for ultra-stable zinc metal anodes

Supplementary files

Article information

Article type
Paper
Submitted
16 May 2024
Accepted
24 Jun 2024
First published
24 Jun 2024

J. Mater. Chem. A, 2024,12, 19060-19068

Elucidating synergistic mechanisms of an anion–cation electrolyte additive for ultra-stable zinc metal anodes

C. Yuan, J. Xiao, C. Liu and X. Zhan, J. Mater. Chem. A, 2024, 12, 19060 DOI: 10.1039/D4TA03414G

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