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A molecular sieve-containing protective separator to suppress the shuttle effect of redox mediators in lithium-oxygen batteries

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Abstract

Lithium-oxygen (Li-O2) batteries have a great potential in energy storage and conversion due to their ultra-high theoretical specific energy, but their applications are hindered by sluggish redox reaction kinetics in the charge/discharge processes. Redox mediators (RMs), as soluble catalysts, are widely used to facilitate the electrochemical processes in the Li-O2 batteries. A drawback of RMs is the shuttle effect due to their solubility and mobility, which leads to the corrosion of a Li metal anode and the degradation of the electrochemical performance of the batteries. Herein, we synthesize a polymer-based composite protective separator containing molecular sieves. The nanopores with a diameter of 4 Å in the zeolite powder (4A zeolite) are able to physically block the migration of 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) molecules with a larger size; therefore, the shuttle effect of TEMPO is restrained. With the assistance of the zeolite molecular sieves, the cycle life of the Li-O2 batteries is significantly extended from ∼ 20 to 170 cycles at a current density of 250 mA·g−1 and a limited capacity of 500 mAh·g−1. Our work provides a highly effective approach to suppress the shuttle effects of RMs and boost the electrochemical performance of Li-O2 batteries.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. U21A2080 and 51788104), Beijing Natural Science Foundation (No. L223008), and National Key Research and Development Program of China (No. 2022YFB2404403).

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  1. Xinbin Wu and Huiping Wu contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China

    Xinbin Wu, Huiping Wu, Shundong Guan, Ying Liang, Kaihua Wen, Ce-Wen Nan & Liangliang Li

  2. High-Tech Institute of Xi’an, Xi’an, 710025, China

    Xinbin Wu, Huanchun Wang & Xuanjun Wang

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  1. Xinbin Wu
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A molecular sieve-containing protective separator to suppress the shuttle effect of redox mediators in lithium-oxygen batteries

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Wu, X., Wu, H., Guan, S. et al. A molecular sieve-containing protective separator to suppress the shuttle effect of redox mediators in lithium-oxygen batteries. Nano Res. 16, 9453–9460 (2023). https://doi.org/10.1007/s12274-023-5663-5

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