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Vol. 17 (2025)

Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes

https://doi.org/10.1007/s40820-025-01774-5
Haoyang Yuan
Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, People’s Republic of China
Wenjun Lin
Laboratory of Advanced Materials, Fudan University, Shanghai 200438, People’s Republic of China
Changhao Tian
Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, People’s Republic of China
Mihaela Buga
ROM‑EST Laboratory, ICSI Energy Department, National Research and Development Institute for Cryogenic and Isotopic Technologies − ICSI, 4 Uzinei, 240050 Ramnicu Valcea, Romania
Tao Huang
Laboratory of Advanced Materials, Fudan University, Shanghai 200438, People’s Republic of China
Aishui Yu
Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, People’s Republic of China

Corresponding Author: Aishui Yu

asyu@fudan.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 288

Abstract

Quasi-solid-state electrolytes, which integrate the safety characteristics of inorganic materials, the flexibility of polymers, and the high ionic conductivity of liquid electrolytes, represent a transitional solution for high-energy-density lithium batteries. However, the mechanisms by which inorganic fillers enhance multiphase interfacial conduction remain inadequately understood. In this work, we synthesized composite quasi-solid-state electrolytes with high inorganic content to investigate interfacial phenomena and achieve enhanced electrode interface stability. Li1.3Al0.3Ti1.7(PO4)3 particles, through surface anion anchoring, improve Li+ transference numbers and facilitate partial dissociation of solvated Li+ structures, resulting in superior ion transport kinetics that achieve an ionic conductivity of 0.51 mS cm−1 at room temperature. The high mass fraction of inorganic components additionally promotes the formation of more stable interfacial layers, enabling lithium-symmetric cells to operate without short-circuiting for 6000 h at 0.1 mA cm−2. Furthermore, this system demonstrates exceptional stability in 5 V-class lithium metal full cells, maintaining 80.5% capacity retention over 200 cycles at 0.5C. These findings guide the role of inorganic interfaces in composite electrolytes and demonstrate their potential for advancing high-voltage lithium battery technology.


Highlights:
1 A high-proportion inorganic composite quasi-solid-state electrolyte was fabricated through the integration of high-speed defoamed mixers with in situ polymerization methodology.
2 The intermediate phase, which exhibits an affinity for anion adsorption, facilitates the partial dissociation of lithium-ion solvation structures, thereby enhancing transport kinetics.
3 The exceptional interfacial stability was demonstrated through a lithium-symmetric cell operating without short-circuiting for 6000 h, while the 5 V-class lithium metal cell maintained 80.5% capacity retention after 200 cycles in 0.5C.

Keywords

Quasi-solid-state electrolytes Lithium metal anode Intermediate phase Na-superionic-conductors 5 V-class cathode
Yuan, Haoyang, Wenjun Lin, Changhao Tian, Mihaela Buga, Tao Huang, and Aishui Yu. 2025. “Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes”. Nano-Micro Letters 17 (June):288. https://doi.org/10.1007/s40820-025-01774-5.
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