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Research Article

A chiral salen-Co(II) complex as soluble redox mediator for promoting the electrochemical performance of Li-O2batteries

Hao Wan1,§, Yingjie Sun2,§, Jia Yu3, Qianqi Shi1, Yongchun Zhu1( ), Yitai Qian1( )
Hefei National Laboratory for Physical Science at Microscale and Department of Chemistry, University of Science and Technology of China, Hefei 230026, China
Hebei Key Laboratory of Photoelectric Control on Surface and Interface, College of Science, Hebei University of Science and Technology, Shijiazhuang 050018, China
Materials Genome Institute, Shanghai University, Shanghai 200444, China

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

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Graphical Abstract

The addition of Co(II) into electrolyte for excellent performance Li-O2 batteries is confirmed. The cell with Co(II) exhibits highly discharge capacity with superior yield of Li2O2 (96.09%) and efficient catalytic for discharge products and by-products, shedding an emerging strategy to achieve large capacity low overpotential long cycle lifespan Li-O2 batteries.

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.

Keywords

chiral salen-Co(II) complexsoluble redox mediatormulti-redox potentialtrifunctionalLi-O2 batteries

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Nano Research
Volume 15 Issue 9,
September 2022
Pages 8101-8108
DOI: 10.1007/s12274-022-4490-4
Cite this article:
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-O2batteries. Nano Research, 2022, 15(9): 8101-8108. https://doi.org/10.1007/s12274-022-4490-4
Topics:
Lithium batteries

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Received: 14 March 2022
Revised: 30 April 2022
Accepted: 02 May 2022
Published: 22 June 2022
© Tsinghua University Press 2022
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