Luo Heming, Yang Jie, Yang Yanfei, Wang Wankai, Han Wenqiang, Zhang Junping
College of Petrochemical Technology, Lanzhou University of Technology, 730050 Lanzhou, P. R. China.
Research Center of Resource Chemistry and Energy Materials, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, 730000 Lanzhou, P. R. China.
ACS Appl Mater Interfaces. 2025 Jun 25;17(25):36763-36772. doi: 10.1021/acsami.5c05964. Epub 2025 Jun 12.
High-performance organic-inorganic composite solid-state electrolytes (OICSEs) are pivotal for advancing solid-state lithium metal batteries (SSLMBs), offering the potential for enhanced safety and higher energy density compared to conventional liquid electrolytes. This study systematically explores the influence of nanofiller physicochemical properties (particle size, specific surface area, and surface energy) on the electrochemical performance of polyethylene oxide (PEO)-based OICSEs. By optimizing these parameters, we developed a PEO/superhydrophobic SiO OICSE incorporating low surface energy SiO nanofillers with an optimized particle size of 7 nm and a high surface area of 300 m g. This engineered OICSE demonstrated exceptional ionic conductivity (4.3 × 10 S cm at 30 °C), high Li-ion transference number (0.5), and superior electrochemical stability (up to 5.1 V vs Li/Li). When integrated into a Li|LiFePO battery, the battery exhibited outstanding rate performance (up to 5.0 C) and remarkable cycling stability (93.8% capacity retention after 500 cycles at 30 °C) and maintained stable performance even at 0 °C. These improvements are attributed to enhanced Li-ion transport pathways and superior solid/solid interfacial stability. The superhydrophobic SiO nanofiller presents a scalable and commercially viable strategy to enhance processability, interfacial compatibility, and low-temperature performance, thereby establishing a robust platform for the development of next-generation OICSEs in SSLMBs.
高性能有机-无机复合固态电解质（OICSEs）对于推进固态锂金属电池（SSLMBs）至关重要，与传统液体电解质相比，具有提高安全性和更高能量密度的潜力。本研究系统地探讨了纳米填料物理化学性质（粒径、比表面积和表面能）对聚环氧乙烷（PEO）基OICSEs电化学性能的影响。通过优化这些参数，我们开发了一种PEO/超疏水SiO OICSE，其包含低表面能的SiO纳米填料，优化粒径为7 nm，高比表面积为300 m²/g。这种工程化的OICSE表现出优异的离子电导率（30℃时为4.3×10⁻⁴ S cm⁻¹）、高锂离子迁移数（0.5）和卓越的电化学稳定性（相对于Li/Li高达5.1 V）。当集成到Li|LiFePO₄电池中时，该电池表现出出色的倍率性能（高达5.0 C）和显著的循环稳定性（30℃下500次循环后容量保持率为93.8%），甚至在0℃时也能保持稳定性能。这些改进归因于增强的锂离子传输途径和优异的固/固界面稳定性。超疏水SiO纳米填料为提高可加工性、界面相容性和低温性能提供了一种可扩展且具有商业可行性的策略，从而为SSLMBs中下一代OICSEs的开发建立了一个强大的平台。
