Improving Ionic Conductivity and Interface Stability in All-Solid-State Batteries Using Nanocomposite Solid Electrolytes
Keywords:
all-solid-state batteries, nanocomposite solid electrolytes, ionic conductivity, interface stability, sol-gel synthesisAbstract
All-solid-state batteries (ASSBs) have emerged as promising candidates for next-generation energy storage due to their intrinsic safety and compatibility with high-energy-density lithium metal anodes. However, their commercialization is hindered by two persistent bottlenecks: the relatively low ionic conductivity of solid electrolytes compared to liquids and the instability of electrode-electrolyte interfaces. Existing approaches often improve one aspect in isolation but fail to simultaneously optimize both properties under practical cycling conditions. In this study, we propose an in situ-assembled nanocomposite solid electrolyte, where oxide nanoparticles are homogeneously dispersed within a sulfide-based host matrix through a sol-gel assisted synthesis. This design integrates percolation pathways that reduce activation energy for Li⁺ transport and introduces a nanoscale passivation layer that suppresses interfacial side reactions. Electrochemical tests demonstrate a room-temperature ionic conductivity of 1.7 × 10⁻³ S·cm⁻¹, a 2.3-fold improvement over pure sulfide and a 6.1-fold improvement over oxide baselines. Interfacial resistance was reduced to 18 Ω·cm², and full-cell cycling retained 91% capacity after 300 cycles. Ablation and robustness studies further confirm the critical role of filler concentration, particle size, and interfacial engineering. These results establish a reproducible framework for enhancing both conductivity and interfacial stability in ASSBs. The proposed nanocomposite design provides a scalable pathway toward safer, high-performance solid-state batteries, directly supporting future applications in electric vehicles and grid-scale energy storage.References
1. S. Antony Jose, A. Gallant, P. L. Gomez, Z. Jaggers, E. Johansson, Z. LaPierre, and P. L. Menezes, "Solid-state lithium batteries: Advances, challenges, and future perspectives," Batteries, vol. 11, no. 3, p. 90, 2025. doi: 10.3390/batteries11030090
2. B. Man, Y. Zeng, Q. Liu, Y. Chen, X. Li, W. Luo, and S. Liu, "A Comprehensive Review of Sulfide Solid-State Electrolytes: Properties, Synthesis, Applications, and Challenges," Crystals, vol. 15, no. 6, p. 492, 2025. doi: 10.3390/cryst15060492
3. Z. Wu, X. Li, C. Zheng, Z. Fan, W. Zhang, H. Huang, and J. Zhang, "Interfaces in sulfide solid electrolyte-based all-solid-state lithium batteries: characterization, mechanism and strategy," Electrochemical Energy Reviews, vol. 6, no. 1, p. 10, 2023. doi: 10.1007/s41918-022-00176-0
4. C. Luo, M. Yi, Z. Cao, W. Hui, and Y. Wang, "Review of ionic conductivity properties of NASICON type inorganic solid electrolyte LATP," ACS Applied Electronic Materials, vol. 6, no. 2, pp. 641-657, 2024. doi: 10.1021/acsaelm.3c01747
5. Y. Nikodimos, W. N. Su, and B. J. Hwang, "Halide solidstate electrolytes: stability and application for high voltage allsolidstate Li batteries," Advanced Energy Materials, vol. 13, no. 3, p. 2202854, 2023.
6. L. Zhao, Y. Li, M. Yu, Y. Peng, and F. Ran, "Electrolytewettability issues and challenges of electrode materials in electrochemical energy storage, energy conversion, and beyond," Advanced Science, vol. 10, no. 17, p. 2300283, 2023. doi: 10.1002/advs.202300283
7. K. Chen, Y. Zhu, J. Li, J. Zhang, H. Luo, S. Yin, and S. Wang, "High Performance Sulfide SolidState Battery Electrolytes Regulation Mechanism: A Review," Angewandte Chemie International Edition, vol. 64, no. 45, p. e202510602, 2025. doi: 10.1002/anie.202510602
8. Z. Cui, and A. Manthiram, "Thermal stability and outgassing behaviors of highnickel cathodes in lithiumion batteries," Angewandte Chemie International Edition, vol. 62, no. 43, p. e202307243, 2023. doi: 10.1002/anie.202307243
9. J. Lei, Z. Wang, Y. Zhang, M. Ju, H. Fei, S. Wang, and J. Wang, "Understanding and resolving the heterogeneous degradation of anion exchange membrane water electrolysis for large-scale hydrogen production," Carbon Neutrality, vol. 3, no. 1, p. 25, 2024. doi: 10.1007/s43979-024-00101-y
10. M. Umair, S. Zhou, W. Li, H. T. H. Rana, J. Yang, L. Cheng, and J. Wei, "Oxide solid electrolytes in solidstate batteries," Batteries & Supercaps, vol. 8, no. 6, p. e202400667, 2025. doi: 10.1002/batt.202400667
11. M. Yang, Y. Yao, M. Chang, F. Tian, W. Xie, X. Zhao, and X. Yao, "High Energy Density SulfurRich MoS6Based Nanocomposite for Room Temperature AllSolidState Lithium Metal Batteries," Advanced Energy Materials, vol. 13, no. 28, p. 2300962, 2023.
12. H. Kwak, J. S. Kim, D. Han, J. S. Kim, J. Park, G. Kwon, and Y. S. Jung, "Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries," Nature communications, vol. 14, no. 1, p. 2459, 2023. doi: 10.1038/s41467-023-38037-z
13. S. Liu, W. Liu, D. Ba, Y. Zhao, Y. Ye, Y. Li, and J. Liu, "Fillerintegrated composite polymer electrolyte for solidstate lithium batteries," Advanced Materials, vol. 35, no. 2, p. 2110423, 2023. doi: 10.1002/adma.202110423
14. M. C. Tekell, G. Nikolakakou, E. Glynos, and S. K. Kumar, "Ionic conductivity and mechanical reinforcement of well-dispersed polymer nanocomposite electrolytes," ACS Applied Materials & Interfaces, vol. 15, no. 25, pp. 30756-30768, 2023. doi: 10.1021/acsami.3c04633
15. S. Liu, L. Zhou, T. Zhong, X. Wu, and K. Neyts, "Sulfide/Polymer Composite SolidState Electrolytes for AllSolidState Lithium Batteries," Advanced Energy Materials, vol. 14, no. 48, p. 2403602, 2024. doi: 10.1002/aenm.202403602
