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Research Article

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

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
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We report a scalable solvent-free strategy for fabricating high ceramic content composite solid-state electrolyte (HCCSE) films. The obtained HCCSE films with 80 wt.% ceramic content exhibit high room temperature ionic conductivity, good mechanical strength, and excellent electrode|electrolyte interfacial stability. As a result, all-solid-state Li metal batteries based on this HCCSE present decent cyclability at 25 °C.

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-standingsolid-state electrolyte filmcomposite solid-state electrolytesolid-state battery

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Nano Research
Volume 16 Issue 3,
March 2023
Pages 3847-3854
DOI: 10.1007/s12274-022-4845-x
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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