J. Am. Chem. Soc. - Dynamical Janus Interface Design for Reversible and Fast-Charging Zinc-Iodine Battery under Extreme Operating Conditions

Wei Zong^¶, Jiantao Li^¶, Chengyi Zhang^¶, Yuhang Dai^¶, Yue Ouyang, Leiqian Zhang, Jianwei Li, Wei Zhang, Ruwei Chen, Haobo Dong, Xuan Gao, Jiexin Zhu, Ivan P. Parkin, Paul R. Shearing, Feili Lai*, Khalil Amine*, Tianxi Liu*, Guanjie He*

J. Am. Chem. Soc. 2024, DOI:10.1021/jacs.4c03615

Aqueous zinc (Zn) iodine (I2) batteries have emerged as viable alternatives to conventional metal-ion batteries. However, undesirable Zn deposition and irreversible iodine conversion during cycling have impeded their progress. To overcome these concerns, we report a dynamical interface design by cation chemistry that improves the reversibility of Zn deposition and four-electron iodine conversion. Due to this design, we demonstrate an excellent Zn-plating/-stripping behavior in Zn||Cu asymmetric cells over 1000 cycles with an average Coulombic efficiency (CE) of 99.95%. Moreover, the Zn||I2 full cells achieve a high-rate capability (217.1 mA h g–1 at 40 A g–1; C rate of 189.5C) at room temperature and enable stable cycling with a CE of more than 99% at −50 °C at a current density of 0.05 A g–1. In situ spectroscopic investigations and simulations reveal that introducing tetraethylammonium cations as ion sieves can dynamically modulate the electrode–electrolyte interface environment, forming the unique water-deficient and chloride ion (Cl–)-rich interface. Such Janus interface accounts for the suppression of side reactions, the prevention of ICl decomposition, and the enrichment of reactants, enhancing the reversibility of Zn-stripping/-plating and four-electron iodine chemistry. This fundamental understanding of the intrinsic interplay between the electrode–electrolyte interface and cations offers a rational standpoint for tuning the reversibility of iodine conversion.

Link: https://pubs.acs.org/doi/10.1021/jacs.4c03615