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Jiajun Cui, Zhenzhen Wang, Yongqiang Gu, Ting Xu, Tairan Pang, Chuanling Si, Weiwei Huan, Jie Li. Single-atom Mn-modified Biomimetic Phthalocyanine Covalent Organic Frameworks with Tunable Pendant Groups for High-efficiency Sodium Chloride Batteries. Green Energy&Environment. doi: 10.1016/j.gee.2025.06.002
Citation: Jiajun Cui, Zhenzhen Wang, Yongqiang Gu, Ting Xu, Tairan Pang, Chuanling Si, Weiwei Huan, Jie Li. Single-atom Mn-modified Biomimetic Phthalocyanine Covalent Organic Frameworks with Tunable Pendant Groups for High-efficiency Sodium Chloride Batteries. Green Energy&Environment. doi: 10.1016/j.gee.2025.06.002
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Single-atom Mn-modified Biomimetic Phthalocyanine Covalent Organic Frameworks with Tunable Pendant Groups for High-efficiency Sodium Chloride Batteries

doi: 10.1016/j.gee.2025.06.002

  • a. College of Chemistry and Materials Engineering, Zhejiang A&F University, Hangzhou, 311300 P. R. China;

  • b. Tianjin Key Laboratory of Pulp and Paper, Tianjin University of Science and Technology, Tianjin 300457, P.R. China;

  • c. Institute of Energy Materials Science (IEMS), University of Shanghai for Science and Technology

Funds:

This work was supported by the National Natural Science Foundation of China (32371809), the Zhejiang Public Welfare Public Research Program (LGC22B010001) and the Fundamental Research Funds for the Provincial University of Zhejiang (2024TD002).

  • Received date 16 April 2025, Accepted date 13 June 2025, RevRecd date 28 May 2025, Available online 20 June 2025
    Abstract
  • Rechargeable chlorine-based battery recently emerged as a promising substitute for energy storage systems due to their high average operating voltage (∼3.7 V) and large theoretical capacity of ∼754.9 mAh g-1. However, insufficient supply of chlorine (Cl2) and sluggish oxidation of NaCl to Cl2 limit its practical application. Covalent Organic Frameworks (COFs) have the potential to be ideal Cl2 host materials as Cl2 adsorbents for their abundant porosity and easily modifiable nature. In this work, the single atom Mn coordinated biomimetic phthalocyanine COFs is used for Cl2 capture and catalyst. The DFT reveals that ASMn and -NH2 significantly change the microenvironment around the active site, effectively promote the oxidation of NaCl. When applied as the cathode material for Na-Cl2 batteries, the SAMn-COFs-NH2 electrode exhibits large reversible capacities and excellent high-rate cycling performances throughout 200 cycles based on the mechanism of highly reversible NaCl/Cl2 redox reactions. Even at the temperature as low as -40 oC, the SAMn-COFs-NH2 cathode showed stable discharge capacities at ∼1000 mAh g-1 over 50 cycles with a voltage plateau of ∼3.3 V. This work may provide new insights for the investigation of chlorine-based electrochemical redox mechanisms and the design of green nanoscaled electrodes for high-property chlorine-based batteries.

     

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