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Nano Research 2023, 16(3): 3847-3854 https://doi.org/10.1007/s12274-022-4845-x
Research Article | Issue | Published: 12 September 2022

High ceramic content composite solid-state electrolyte films prepared via a scalable solvent-free process

Show Author's Information Daiqian Chen1,2,  Chenji Hu2,3,  Qi Chen4,  Guoyong Xue2,  Lingfei Tang2,  Qingyu Dong2,  Bowen Chen2,  Fengrui Zhang2,  Mingwen Gao4,  Jingjing Xu2,  Yanbin Shen2( ),  Liwei Chen1,2,3
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou 215123, China
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, and in situ Center for Physical Sciences, Shanghai Jiao Tong University, Shanghai 200240, China
Baosheng (Suzhou) Energy Technology Co., Ltd, Suzhou 215123, China
Keywords:
free-standing, solid-state battery, composite solid-state electrolyte, solid-state electrolyte film
Topics:
State Batteries
Cite this article:
Chen D, Hu C, Chen Q, et al. High ceramic content composite solid-state electrolyte films prepared via a scalable solvent-free process. Nano Research, 2023, 16(3): 3847-3854. https://doi.org/10.1007/s12274-022-4845-x
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Abstract Full text Electronic supplementary material About this article

The development of high-performance solid-state electrolyte (SSE) films is critical to the practical application of all-solid-state Li metal batteries (ASSLMBs). However, developing high-performance free-standing electrolyte films remains a challenging task. In this work, we demonstrate a novel scalable solvent-free process for fabricating high ceramic content composite solid-state electrolyte (HCCSE) films. Specifically speaking, a mixture of ceramic and polymer is dry mixed, fibered, and calendered into a free-standing porous ceramic film, on which polymer precursor is coated and polymerized to bridge the inorganic ceramic particles, resulting in a flexible HCCSE film with a ceramic content of up to 80 wt.%. High ceramic content not only leads to high ionic conductivity but also brings good mechanical properties; while the organic phase enables electrode|electrolyte interfacial stability. When Li10GeP2S12 (LGPS) and polymeric ionic liquid-based solid polymer electrolytes (PIL-SPEs) were used as the inorganic and organic phases, respectively, the room temperature ionic conductivity of the resulted HCCSE reaches 0.91 mS·cm−1. Based on this HCCSE, Li||Li symmetric battery cycled stably for more than 2,400 h with ultra-low overpotential, and ASSLMBs with different cathodes (LiFePO4 and sulfurized polyacrylonitrile (PAN-S)) present small polarization and decent cyclability at room temperature. This work provides a novel scalable solvent-free strategy for preparing high-performance free-standing composite solid-state electrolyte (CSE) film for room temperature ASSLMBs.


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Electronic supplementary material
About this article

High ceramic content composite solid-state electrolyte films prepared via a scalable solvent-free process

Show Author's information Daiqian Chen1,2, Chenji Hu2,3, Qi Chen4, Guoyong Xue2, Lingfei Tang2, Qingyu Dong2, Bowen Chen2, Fengrui Zhang2, Mingwen Gao4, Jingjing Xu2, Yanbin Shen2( ), Liwei Chen1,2,3
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou 215123, China
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, and in situ Center for Physical Sciences, Shanghai Jiao Tong University, Shanghai 200240, China
Baosheng (Suzhou) Energy Technology Co., Ltd, Suzhou 215123, China

Abstract

The development of high-performance solid-state electrolyte (SSE) films is critical to the practical application of all-solid-state Li metal batteries (ASSLMBs). However, developing high-performance free-standing electrolyte films remains a challenging task. In this work, we demonstrate a novel scalable solvent-free process for fabricating high ceramic content composite solid-state electrolyte (HCCSE) films. Specifically speaking, a mixture of ceramic and polymer is dry mixed, fibered, and calendered into a free-standing porous ceramic film, on which polymer precursor is coated and polymerized to bridge the inorganic ceramic particles, resulting in a flexible HCCSE film with a ceramic content of up to 80 wt.%. High ceramic content not only leads to high ionic conductivity but also brings good mechanical properties; while the organic phase enables electrode|electrolyte interfacial stability. When Li10GeP2S12 (LGPS) and polymeric ionic liquid-based solid polymer electrolytes (PIL-SPEs) were used as the inorganic and organic phases, respectively, the room temperature ionic conductivity of the resulted HCCSE reaches 0.91 mS·cm−1. Based on this HCCSE, Li||Li symmetric battery cycled stably for more than 2,400 h with ultra-low overpotential, and ASSLMBs with different cathodes (LiFePO4 and sulfurized polyacrylonitrile (PAN-S)) present small polarization and decent cyclability at room temperature. This work provides a novel scalable solvent-free strategy for preparing high-performance free-standing composite solid-state electrolyte (CSE) film for room temperature ASSLMBs.

Keywords: free-standing, solid-state battery, composite solid-state electrolyte, solid-state electrolyte film

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Publication history
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Acknowledgements

Publication history

Received: 18 April 2022
Revised: 30 July 2022
Accepted: 01 August 2022
Published: 12 September 2022
Issue date: March 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 21733012 and 22179143) and the National Key R&D Program of China (No. 2021YFB3800300). We acknowledge Vacuum Interconnected Nanotech Workstation (Nano-X), Suzhou Institute of Nano-Tech and Nano-Bionics for the support in XPS characterization.

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