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Research Article

Manipulating dielectric property of polymer coatings toward high-retention-rate lithium metal full batteries under harsh critical conditions

Qi Kang1, Zechao Zhuang2, Yong Li3, Yinze Zuo4, Jian Wang5, Yijie Liu1, Chaoqun Shi6, Jie Chen1, Hongfei Li1, Pingkai Jiang1, Xingyi Huang1( )
Department of Polymer Science and Engineering, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, Bremen 28359, Germany
Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, China
Helmholtz Institute Ulm (HIU), Ulm D89081, Germany
School of Electrical Engineering, Xi’an Jiaotong University, Xi’an 710049, China
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Graphical Abstract

The dielectric polymer coatings for controlling the deposition of Li and affect the performance of full cells were analyzed in detail. Density functional theory (DFT) calculation and COMSOL simulation demonstrate the power of dielectric polarity of polymer coating in the depth of atomic scale. Li metal full cell with a high-retention-rate of 97.0% after 200 cycles is realized at a high NCM523 loading of 18.69 mg∙cm−2 and a low N/P ratio of 1.6.

Abstract

Lithium (Li) metal batteries (LMBs) can potentially deliver much higher energy density but remain plagued by uncontrollable Li plating with dendrite growth, unstable interfaces, and highly abundant excess Li (> 50 mAh∙cm−2). Herein, different from the artificial layer or three-dimensional (3D) matrix host constructions, various dielectric polymers are initially well-comprehensively investigated from experimental characterizations to theoretical simulation to evaluate their functions in modulating Li ion distribution. As a proof of concept, a 3D interwoven high dielectric functional polymer (HDFP) nanofiber network with polar C–F dipole moments electrospun on copper (Cu) foil is designed, realizing uniform and controllable Li deposition capacity up to 5.0 mAh∙cm−2, thereby enabling stable Li plating/stripping cycling over 1400 h at 1.0 mA∙cm−2. More importantly, under the high-cathode loading (~ 3.1 mAh∙cm−2) and only 0.6 × excess Li (N/P ratio of 1.6), the full cells retain capacity retention of 97.4% after 200 cycles at 3.36 mA∙cm−2 and achieve high energy density (297.7 Wh∙kg−1 at cell-level) under lean electrolyte conditions (15 μL), much better than ever-reported literatures. Our work provides a new direction for designing high dielectric polymer coating toward high-retention-rate practical Li full batteries.

Keywords

high dielectric functional polymernanofiberLi metal full celllow N/P ratiohigh-retention capacity

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Nano Research
Volume 16 Issue 7,
July 2023
Pages 9240-9249
DOI: 10.1007/s12274-023-5478-4
Cite this article:
Kang Q, Zhuang Z, Li Y, et al. Manipulating dielectric property of polymer coatings toward high-retention-rate lithium metal full batteries under harsh critical conditions. Nano Research, 2023, 16(7): 9240-9249. https://doi.org/10.1007/s12274-023-5478-4
Topics:
Lithium batteries

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Received: 12 December 2022
Revised: 04 January 2023
Accepted: 05 January 2023
Published: 19 February 2023
© Tsinghua University Press 2023
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