Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-s...Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.展开更多
文摘Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.
