4.8 Article

Physicochemical Confinement Effect Enables High-Performing Zinc-Iodine Batteries

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 47, Pages 21683-21691

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c09445

Keywords

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Funding

  1. National Natural Science Foundation of China [22175108]
  2. Natural Scientific Foundation [ZR2020JQ09]
  3. Taishan Scholars Program of Shandong Province
  4. Project for Scientific Research Innovation Team of Young Scholars in Colleges, Universities of Shandong Province [2019KJC025]

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This study demonstrates the enhancement of physicochemical confinement effect and electrocatalytic redox conversion of iodine in zinc-iodine batteries by embedding a single iron atom in porous carbon with a metal-nitrogen-carbon bridging structure, which is crucial for fabricating high-performing batteries.
Zinc-iodine batteries are promising energy storage devices with the unique features of aqueous electrolytes and safer zinc. However, their performances are still limited by the polyiodide shuttle and the unclear redox mechanism of iodine species. Herein, a single iron atom was embedded in porous carbon with the atomic bridging structure of metal-nitrogen-carbon to not only enhance the confinement effect but also invoke the electrocatalytic redox conversion of iodine, thereby enabling the large capacity and good cycling stability of the zinc-iodine battery. In addition to the physical trapping effect of porous carbon with good electronic conductivity, the in situ experimental characterization and theoretical calculation reveal that the metal-nitrogen-carbon bridging structure modulates the electronic properties of carbon and adjusts the intrinsic activity for the reversible conversion of iodine via the thermodynamically favorable pathway. This work demonstrates that the physicochemical confinement effect can be invoked by the rational anchoring of a single metal atom with nitrogen in a porous carbon matrix to enhance the electrocatalytic redox conversion of iodine, which is crucial to fabricating high-performing zinc-iodine batteries and beyond by applying the fundamental principles.

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