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Dynamical Janus Interface Design for Reversible and Fast-Charging Zinc–Iodine Battery under Extreme Operating Conditions

Zong, Wei; Li, Jiantao; Zhang, Chengyi; Dai, Yuhang; Ouyang, Yue; Zhang, Leiqian; Li, Jianwei; ... He, Guanjie; + view all (2024) Dynamical Janus Interface Design for Reversible and Fast-Charging Zinc–Iodine Battery under Extreme Operating Conditions. Journal of the American Chemical Society , 146 (31) pp. 21377-21388. 10.1021/jacs.4c03615.

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Abstract

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.

Type: Article
Title: Dynamical Janus Interface Design for Reversible and Fast-Charging Zinc–Iodine Battery under Extreme Operating Conditions
Location: United States
DOI: 10.1021/jacs.4c03615
Publisher version: https://doi.org/10.1021/jacs.4c03615
Language: English
Additional information: This version is the author-accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10196135
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