Unlocking Durable and Sustainable Zinc–Iodine Batteries via Molecularly Engineered Polyiodide Reservoirs
Abstract
Abstract Zinc–iodine batteries (ZIBs) are promising candidates for safe and sustainable energy storage but are hindered by polyiodide shuttling, leading to rapid capacity decay and limited cyclability. In this work, we propose a “polyiodide reservoirs” concept, utilizing iodophilic covalent organic cages to confine polyiodide through multiple noncovalent interactions. By precisely engineering the nitrogen‐active site densities around 3D cavities, these cages evolve from open to near‐enclosed structure, achieving molecular‐level polyiodide entrapment. The optimized superphane cage (18 N‐active sites) enables a ZIB with 90.1% capacity retention after 4000 cycles at 5 C, even under extreme conditions (58.9 wt% iodine content within the cage and an iodine area loading of 3.7 mg cm −2 in the cathode). Importantly, the cage's solubility‐driven regeneration capability retains 85.4% initial capacity over three reuse cycles. This work establishes covalent organic superphanes as a transformative platform for long‐life ZIBs, offering a dual solution to shuttle suppression and electrode sustainability through structural confinement and dynamic recyclability.
Article Details
Authors (14)
Leiqian Zhang
Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University Wuxi 214122 P.R. China
Ke Luo
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering
Jiaming Gong
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 P.R. China
Yazhou Zhou
Institute of Physics, Chinese Academy of Sciences
Hele Guo
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites
Yi Yu
Guanjie He
Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
Jean‐François Gohy
Institute of Condensed Matter and Nanoscience (IMCN) Université catholique de Louvain Place L. Pasteur 1 Louvain‐la‐Neuve 1348 Belgium
Ivan P. Parkin
Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
Johan Hofkens
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium
Qing He
Tianxi Liu
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering
Klaus Müllen
Feili Lai
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium