Organocatalytic Lithium Chloride Oxidation by Covalent Organic Frameworks for Rechargeable Lithium-Chlorine Batteries

Yan Xu; Mingming Wang; Muhammad Sajid; Yahan Meng; Zehui Xie; Lidong Sun; Jian Jin; Wei Chen; Shenxiang Zhang

doi:10.1002/anie.202315931

Organocatalytic Lithium Chloride Oxidation by Covalent Organic Frameworks for Rechargeable Lithium-Chlorine Batteries

Angew Chem Int Ed Engl. 2024 Feb 12;63(7):e202315931. doi: 10.1002/anie.202315931. Epub 2023 Dec 18.

Authors

Yan Xu^{1

2}, Mingming Wang², Muhammad Sajid², Yahan Meng², Zehui Xie², Lidong Sun², Jian Jin³, Wei Chen², Shenxiang Zhang³

Affiliations

¹ College of Energy, Soochow Institute for Energy and Materials Innovations, Light Industry Institute of Electrochemical Power Sources, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, Jiangsu 215006, China.
² Department of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
³ College of Chemistry, Chemical Engineering and Materials Science, Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, Jiangsu 215123, China.

PMID: 38050465
DOI: 10.1002/anie.202315931

Abstract

Rechargeable Li-Cl₂ battery is a promising high energy density battery system. However, reasonable cycle life could only be achieved under low specific capacities due to the sluggish oxidation of LiCl to Cl₂ . Herein, we propose an amine-functionalized covalent organic framework (COF) with catalytic activity, namely COF-NH₂ , that significantly decreases the oxidation barrier of LiCl and accelerates the oxidation kinetics of LiCl in Li-Cl₂ cell. The resulting Li-Cl₂ cell using COF-NH₂ (Li-Cl₂ @COF-NH₂ ) simultaneously exhibits low overpotential, ultrahigh discharge capacity up to 3500 mAh/g and a promoted utilization ratio of deposited LiCl at the first cycle (UR-LiCl) of 81.4 %, which is one of the highest reported values to date. Furthermore, the Li-Cl₂ @COF-NH₂ cell could be stably cycled for over 200 cycles when operating at a capacity of 2000 mAh/g at -20 °C with a Coulombic efficiency (CE) of ≈100 % and a discharge plateau of 3.5 V. Our superior Li-Cl₂ batteries enabled by organocatalyst enlighten an arena towards high-energy storage applications.

Keywords: Covalent Organic Framework; High Energy Density; Lithium Chloride Oxidation; Lithium-Chlorine Battery; Organocatalysis.

Abstract

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