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Polymer matrix mediated solvation of LiNO3 in carbonate electrolytes for quasi-solid high-voltage lithium metal batteries

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Abstract

Lithium (Li) metal is one of the most promising anodes for next-generation energy storage systems. However, the Li dendrite formation and unstable solid-electrolyte interface (SEI) have hindered its further application. Lithium nitrate (LiNO3) is extensively used as an effective electrolyte additive in ether-based electrolytes to improve the stability of lithium metal. Nevertheless, it is rarely utilized in carbonate electrolytes due to its low solubility. Here, a novel gel polymer electrolyte (GPE) consisting of poly(vinylidene fluoride) (PVDF), poly(methyl methacrylate) (PMMA), poly(ethylene oxide) (PEO) with LiNO3 additive is proposed to solve this issue. In this GPE, polyether-based PEO serves as a matrix for dissolving LiNO3 which can be decomposed into a fast Li-ion conductor (Li3N) in conventional carbonate electrolytes to enhance the stability and Li+ conductivity of the SEI film. As a result, dendrite formation is effectively suppressed, and a significantly improved average Coulombic efficiency (CE) of 97.2% in Li-Cu cell is achieved. By using this novel GPE coupled with Li anode and LiNi0.5Mn0.3Co0.2O2 (NMC532), excellent capacity retention of 94.1% and high average CE of over 99.2% are obtained after 200 cycles at 0.5 C. This work presents fresh insight into practical modification strategies on high-voltage Li metal batteries.

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Acknowledgements

This work was financially supported by National Key R&D Program of China (No. 2016YFB0700600), Soft Science Research Project of Guangdong Province (No. 2017B030301013), and Shenzhen Science and Technology Research Grant (No. ZDSYS201707281026184).

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Authors and Affiliations

  1. School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, China

    Zijian Wang, Kai Yang, Yongli Song, Hai Lin, Ke Li, Yanhui Cui, Luyi Yang & Feng Pan

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  1. Zijian Wang
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Correspondence to Luyi Yang or Feng Pan.

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12274_2020_2871_MOESM1_ESM.pdf

Polymer matrix mediated solvation of LiNO3 in carbonate electrolytes for quasi-solid high-voltage lithium metal batteries

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Wang, Z., Yang, K., Song, Y. et al. Polymer matrix mediated solvation of LiNO3 in carbonate electrolytes for quasi-solid high-voltage lithium metal batteries. Nano Res. 13, 2431–2437 (2020). https://doi.org/10.1007/s12274-020-2871-0

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