Compatibility Integrated Sulfide‐Based Cathode and Electrolyte for High‐Energy Solid‐State Sodium Batteries <sup>†</sup>

Xu, Hewei;Lin, Xiaodong;Chang, Hong;Apostol, Petru;Vlad, Alexandru;et.al.
(2025) Chinese Journal of Chemistry — Vol. 44, n° 1, p. 73-79 (2025)

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Authors
  • Xu, HeweiUCLouvain
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  • Lin, Xiaodongorcid-logoUCLouvain
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  • Chang, Hong
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  • Wang, JiandeUCLouvain
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  • Liu, XuelianUCLouvain
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  • Zhang, XiaozheUCLouvain
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  • Tie, DaUCLouvain
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Abstract
The scarcity of critical raw materials in lithium-ion batteries has driven increasing interest in alternative chemistries, such as sodium- based all-solid-state batteries. Among various solid electrolytes, sulfide-based Na3PS4 stands out for its high ionic conductivity and excellent formability. However, its poor interfacial compatibility with conventional high-voltage oxide cathodes remains a major limitation. In this study, we report the successful integration of amorphous Na2MoS4—a high-capacity, sulfide-compatible cathode—into Na3PS4-based all-solid-state sodium batteries. Benefiting from a moderate redox potential window (1.1–2.7 V vs. Na+/Na), Na2MoS4 exhibits excellent chemical and electrochemical compatibility with Na3PS4, as confirmed by structural and spectroscopic analyses. Further investigation reveals that intimate interfacial contact between both electrodes and the solid-state electrolyte is critical for achieving long-term cycling stability. Based on these insights, the optimized Na15Sn4 | Na3PS4 | Na2MoS4-Na3PS4-carbon nanofiber cell delivers a reversible capacity of ~372 mAh·g–1 at 0.1 C and retains nearly 100% capacity over 450 cycles at 0.3 C. In situ impedance spectroscopy further confirms the stability of interfacial resistance throughout cycling. This work identifies Na2MoS4 as a highly promising sulfide cathode for high-energy, long-life sodium solid-state batteries and provides valuable design principles for future development of sulfide-based electrode-electrolyte interfaces in next-generation energy storage systems.
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Xu, H., Lin, X., Chang, H., Apostol, P., Wang, J., Liu, X., Zhang, X., Tie, D., & Vlad, A. (2025). Compatibility Integrated Sulfide‐Based Cathode and Electrolyte for High‐Energy Solid‐State Sodium Batteries <sup>†</sup> Chinese Journal of Chemistry, 44(1), 73-79. https://doi.org/10.1002/cjoc.70313 (Original work published 2025)