Key Takeaways & Executive Findings
- •• A high-proportion inorganic composite quasi-solid-state electrolyte was fabricated via high-speed defoamed mixers and in situ polymerization, achieving enhanced ionic conductivity of 0.51 mS cm−1 at room temperature. • The intermediate phase, with anion-adsorbing affinity, facilitates partial dissociation of lithium-ion solvation structures, improving Li+ transport kinetics and transference numbers. • Exceptional interfacial stability is demonstrated by lithium-symmetric cells operating without short-circuiting for 6000 h at 0.1 mA cm−2. • The system maintains 80.5% capacity retention after 200 cycles at 0.5C in 5 V-class lithium metal full cells, highlighting its potential for high-voltage applications.
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.
1. Introduction
With an extraordinarily high specific capacity (3860 mAh g−1) and remarkably low reduction potential (−3.04 V versus standard hydrogen electrode), lithium metal anodes contribute to the potential for achieving high energy density storage solutions that are crucial for next-generation clean energy storage systems [1–3]. However, the implementation of lithium metal anodes presents significant technical challenges, primarily stemming from their inherent high chemical reactivity. This reactivity poses substantial challenges for maintaining stable interfaces within the battery system. Traditional liquid electrolytes, despite their widespread use, carry inherent risks due to their toxicity and volatility [4]. In contrast, solid-state electrolytes serve as a safety enhancement through their ability to delay thermal runaway [5, 6].
When examining ionic conductivity at room temperature, these materials follow a hierarchical order: polymer electrolytes [7, 8], followed by oxides [9, 10], chlorides [11, 12], and sulfides [13, 14]. Polymer electrolytes, while benefiting from mechanical flexibility that aids in maintaining intimate electrode contact, are constrained by their relatively low ionic conductivity [8, 15]. Oxide electrolytes stand out for their superior thermodynamic stability, though their effectiveness is hampered by high grain boundary resistance that impedes ion transport [16]. Chlorides, despite their great conductivity, face compatibility challenges with lithium metal anodes, limiting their practical application [17, 18]. Sulfide electrolytes achieve the highest ionic conductivity among these categories but suffer from poor thermodynamic stability, making them vulnerable to decomposition [19, 20].
These inherent limitations inspired researchers to pursue composite approaches, combining different electrolyte types to create systems that capitalize on their complementary strengths while mitigating their weaknesses. One strategy involves incorporating inorganic particles as fillers within polymer matrices. This approach predominantly focused on materials like Na-superionic-conductor (NASICON) LATP (Li1.3Al0.3Ti1.7(PO4)3) [21, 22], LAGP (Li1.5Al0.5Ge1.5(PO4)3) [23], and garnet LLZTO (Li6.5La3Zr1.5Ta0.5O12) [24], chosen for their excellent thermodynamic stability and relatively straightforward synthesis procedures. Nevertheless, the ionic conductivity of oxide–polymer composite solid-state electrolytes remains
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Haoyang Yuan, Wenjun Lin, Changhao Tian, Mihaela Buga, Tao Huang, Aishui Yu (2025). Enhancement of Li+ Transport Through Intermediate Phase in High-Content Inorganic Composite Quasi-Solid-State Electrolytes. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01774-5
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Frequently Asked Questions
What is the main achievement of this study?
The study demonstrates a high-content inorganic composite quasi-solid-state electrolyte that achieves enhanced Li+ transport through an intermediate phase, resulting in high ionic conductivity (0.51 mS cm−1) and exceptional interfacial stability, enabling 6000 h of lithium-symmetric cell operation and 80.5% capacity retention after 200 cycles in 5 V-class full cells.
How does the intermediate phase enhance Li+ transport?
The intermediate phase, formed by LATP particles, exhibits anion-adsorbing affinity, which facilitates partial dissociation of lithium-ion solvation structures, thereby improving Li+ transference numbers and overall transport kinetics.
What is the significance of the 6000 h lithium-symmetric cell test?
The 6000 h operation without short-circuiting demonstrates exceptional interfacial stability, indicating that the composite electrolyte effectively suppresses lithium dendrite growth and maintains a stable electrode-electrolyte interface.
What are the potential applications of this electrolyte?
This quasi-solid-state electrolyte is suitable for high-energy-density lithium metal batteries, particularly those requiring high-voltage operation (5 V-class cathodes), offering improved safety and long cycle life.
What is the role of inorganic fillers in the composite electrolyte?
Inorganic fillers like LATP enhance ionic conductivity by promoting partial dissociation of Li+ solvation structures and improving Li+ transference numbers. They also contribute to the formation of stable interfacial layers, improving overall battery performance.
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