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Vol. 17 (2025)

Host–Guest Inversion Engineering Induced Superionic Composite Solid Electrolytes for High-Rate Solid-State Alkali Metal Batteries

https://doi.org/10.1007/s40820-025-01691-7
Xiong Xiong Liu
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Long Pan
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Haotian Zhang
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Pengcheng Yuan
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Mufan Cao
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Yaping Wang
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Zeyuan Xu
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Min Gao
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Zheng Ming Sun
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China

Corresponding Author: Zheng Ming Sun

zmsun@seu.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 190

Abstract

Composite solid electrolytes (CSEs) are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost due to expensive active ceramic fillers. Here, a host–guest inversion engineering strategy is proposed to develop superionic CSEs using cost-effective SiO2 nanoparticles as passive ceramic hosts and poly(vinylidene fluoride-hexafluoropropylene) (PVH) microspheres as polymer guests, forming an unprecedented “polymer guest-in-ceramic host” (i.e., PVH-in-SiO2) architecture differing from the traditional “ceramic guest-in-polymer host”. The PVH-in-SiO2 exhibits excellent Li-salt dissociation, achieving high-concentration free Li+. Owing to the low diffusion energy barriers and high diffusion coefficient, the free Li+ is thermodynamically and kinetically favorable to migrate to and transport at the SiO2/PVH interfaces. Consequently, the PVH-in-SiO2 delivers an exceptional ionic conductivity of 1.32 × 10−3 S cm−1 at 25 °C (vs. typically 10−5–10−4 S cm−1 using high-cost active ceramics), achieved under an ultralow residual solvent content of 2.9 wt% (vs. 8–15 wt% in other CSEs). Additionally, PVH-in-SiO2 is electrochemically stable with Li anode and various cathodes. Therefore, the PVH-in-SiO2 demonstrates excellent high-rate cyclability in LiFePO4|Li full cells (92.9% capacity-retention at 3C after 300 cycles under 25 °C) and outstanding stability with high-mass-loading LiFePO4 (9.2 mg cm−1) and high-voltage NCM622 (147.1 mAh g−1). Furthermore, we verify the versatility of the host–guest inversion engineering strategy by fabricating Na-ion and K-ion-based PVH-in-SiO2 CSEs with similarly excellent promotions in ionic conductivity. Our strategy offers a simple, low-cost approach to fabricating superionic CSEs for large-scale application of solid-state Li metal batteries and beyond.


Highlights:
1 Host–guest inversion engineering is proposed to create poly(vinylidene fluoride-hexafluoropropylene) (PVH)-in-SiO2 composite solid electrolytes with an original “polymer guest-in-ceramic host” architecture, exhibiting optimized interfacial contacts and comprehensive properties.
2 The PVH-in-SiO2 exhibits an overwhelming ionic conductivity of 1.32 × 10−3 S cm−1 at 25 °C, with an ultralow residual solvent content of 2.9 wt%. In addition, the LiFePO4|PVH-in-SiO2|Li full cells deliver a significant capacity retention of 92.9% at an ultrahigh rate of 3C after 300 cycles at 25 °C.
3 The host–guest inversion engineering is a versatile strategy, as proved by preparing Na+ and K+-based PVH-in-SiO2 composite solid electrolytes, delivering excellent ionic conductivity of 10−4 S cm−1 at 25 °C (vs. 10−6–10−5 S cm−1 of previous reports).

Keywords

Host–guest inversion engineering SiO2 nanoparticle Superionic conductivity Composite solid electrolyte Solid-state alkali metal battery
Liu, Xiong Xiong, Long Pan, Haotian Zhang, Pengcheng Yuan, Mufan Cao, Yaping Wang, Zeyuan Xu, Min Gao, and Zheng Ming Sun. 2025. “Host–Guest Inversion Engineering Induced Superionic Composite Solid Electrolytes for High-Rate Solid-State Alkali Metal Batteries”. Nano-Micro Letters 17 (March):190. https://doi.org/10.1007/s40820-025-01691-7.
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