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.
Text
Parkin_Accepted-JACS_MS 0822.pdf Access restricted to UCL open access staff until 25 July 2025. Download (29MB) |
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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