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A chiral salen-Co(II) complex as soluble redox mediator for promoting the electrochemical performance of Li-O2 batteries

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Abstract

Low discharge capacity and poor cycle stability are the major obstacles hindering the operation of Li-O2 batteries with high-energy-density. These obstacles are mainly caused by the cathode passivation behaviours and the accumulation of by-products. Promoting the discharge process in solution and accelerating the decomposition of discharge products and by-products are able to alleviate above problems to some extent. Herein, chiral salen-Co(II) complex, (1R,2R)-(-)-N,N-bis(3,5-di-t-butylsalicylidene)-1,2-cyclohexanediaminocobalt(II) (Co(II)) as a multi-functional redox mediator was introduced into electrolyte to induce solution phase formation of Li2O2 and catalyze the oxidation of Li2O2 and main by-products Li2CO3. Due to the Co(II) has the solvation effect towards Li+, it can drive solution phase formation of Li2O2, to prevent electrode from passivation and then increase the discharge capacity with a high Li2O2 yield of 96.09 %. Furthermore, the Co(II) possesses suitable redox couple potentials, and it does so while simultaneously boosting the oxidization of Li2O2 and the decomposition of Li2CO3, reducing charge overpotential, and promoting cycle lifespan. Thereby, a cell with Co(II) achieved a long cycling stability at low charge plateau (3.66 V) over 252 cycles with a specific capacity of 500 mAh·gcarbon−1.

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Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (No. 2017YFA0206703), the National Natural Science Foundation of China (No. 22075270), the National Natural Science Foundation of China (No. 21903019), and the Top Young Talents Program in University of Hebei Province (No. BJ2020014), and the numerical calculations in this paper have been done on the supercomputing system in the Supercomputing Center of University of Science and Technology of China.

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  1. Hao Wan and Yingjie Sun contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory for Physical Science at Microscale and Department of Chemistry, University of Science and Technology of China, Hefei, 230026, China

    Hao Wan, Qianqi Shi, Yongchun Zhu & Yitai Qian

  2. Hebei Key Laboratory of Photoelectric Control on Surface and Interface, College of Science, Hebei University of Science and Technology, Shijiazhuang, 050018, China

    Yingjie Sun

  3. Materials Genome Institute, Shanghai University, Shanghai, 200444, China

    Jia Yu

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  1. Hao Wan
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Correspondence to Yongchun Zhu or Yitai Qian.

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A chiral salen-Co(II) complex as soluble redox mediator for promoting the electrochemical performance of Li-O2 batteries

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Wan, H., Sun, Y., Yu, J. et al. A chiral salen-Co(II) complex as soluble redox mediator for promoting the electrochemical performance of Li-O2 batteries. Nano Res. 15, 8101–8108 (2022). https://doi.org/10.1007/s12274-022-4490-4

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