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 N...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 Na_(3)PS_(4) 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 Na_(2)MoS_(4)—a high-capacity,sulfide-compatible cathode—into Na_(3)PS_(4)-based all-solid-state sodium batteries.Benefiting from a moderate redox potential window(1.1-2.7 V vs.Na^(+)/Na),Na_(2)MoS_(4) exhibits excellent chemical and electrochemical compatibility with Na_(3)PS_(4),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 Na_(15)Sn_(4)|Na_(3)PS_(4)|Na_(2)MoS_(4)-Na_(3)PS_(4)-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 Na_(2)MoS_(4) 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.展开更多
基金supported by Taiyuan Institute of Technology Scientific Research Initial Funding(2024KLO06,2024LJ002,2024KJ037)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2024L365)+5 种基金Fund Program for the Scientific Activities of Selected Returned Overseas Professionals in Shanxi Province(20240031)Shanxi Provincial Research Foundation for Basic Research(20210302124219)H.X.,J.W.,X.L.,and X.Z.acknowledge China Scholarship Council for funding.X.L.acknowledges financial support from the Marie Sktodowska-Curie Actions(grant agreement No.101064286)the Fonds de la Recherche Scientifique-FNRs(Grant No.40010559)for his postdoctoral fellowshipAlexandru Vlad acknowledges financial support by INNOVIRIS 2019-RDIR-59B,INNOVIRIS 2O24-RDIR-43B,F.R.S.-FNRS thrOugh grant No°-F.4552.21-DEMIST,CF-ARC grant(18/23-093)MICROBAT,FWOF.R.S.-FNRS under the Excellence of Science(EOS)program-ECOBAT[40007515].
文摘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 Na_(3)PS_(4) 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 Na_(2)MoS_(4)—a high-capacity,sulfide-compatible cathode—into Na_(3)PS_(4)-based all-solid-state sodium batteries.Benefiting from a moderate redox potential window(1.1-2.7 V vs.Na^(+)/Na),Na_(2)MoS_(4) exhibits excellent chemical and electrochemical compatibility with Na_(3)PS_(4),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 Na_(15)Sn_(4)|Na_(3)PS_(4)|Na_(2)MoS_(4)-Na_(3)PS_(4)-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 Na_(2)MoS_(4) 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.
