The development of electrolytes with high ionic conductivity and stable electrode–electrolyte interfaces is crucial for the practical realization of solid-state sodium batteries.In this study,the effect of heteroatom...The development of electrolytes with high ionic conductivity and stable electrode–electrolyte interfaces is crucial for the practical realization of solid-state sodium batteries.In this study,the effect of heteroatom doping in a von-Alpen-type Na super ionic conductor(NASICON)was investigated by substituting Zr^(4+)with Mg^(2+),Zn^(2+),and La^(3+)to enhance its material properties and evaluate its potential for solid-state sodium battery applications.Computational chemistry was employed to predict the thermodynamic stability influenced by dopant introduction and the changes in ionic conductivity arising from crystal structure distortion,with the predictions validated by experiments.The optimized Zn^(2+)-doped NASICON(Zn-NZSP0.07)exhibited the highest total ionic conductivity of 2.74×10^(−3)S∙cm^(−1),representing a 4.5-fold increase compared with undoped NASICON(6.00×10−4 S∙cm^(−1)).The material also showed a high relative density of 99.1%,indicating a compact and well-sintered microstructure,as confirmed by a three-point bending test.Furthermore,a high critical current density of 1.4 mA∙cm^(−2)was achieved in symmetric cell testing.Additionally,a Na_(3)V_(2)(PO_(4))_(3)||Zn-NZSP0.07||Na cell delivered an initial capacity of 103.9 mAh∙g^(−1)at 0.1 A∙g^(−1)and retained 73.4%of its capacity after 200 cycles.These results demonstrate that optimal heteroatom doping is crucial for enhancing the performance of NASICON.展开更多
基金supported by Korea Research Institute for defense Technology planning and advancement(KRIT)grant funded by the Korea government(Defense Acquisition Program Administration(DAPA))(No.21-107-D00-009,Design and development of core materials and unit cells for seawater secondary batteries,2025).
文摘The development of electrolytes with high ionic conductivity and stable electrode–electrolyte interfaces is crucial for the practical realization of solid-state sodium batteries.In this study,the effect of heteroatom doping in a von-Alpen-type Na super ionic conductor(NASICON)was investigated by substituting Zr^(4+)with Mg^(2+),Zn^(2+),and La^(3+)to enhance its material properties and evaluate its potential for solid-state sodium battery applications.Computational chemistry was employed to predict the thermodynamic stability influenced by dopant introduction and the changes in ionic conductivity arising from crystal structure distortion,with the predictions validated by experiments.The optimized Zn^(2+)-doped NASICON(Zn-NZSP0.07)exhibited the highest total ionic conductivity of 2.74×10^(−3)S∙cm^(−1),representing a 4.5-fold increase compared with undoped NASICON(6.00×10−4 S∙cm^(−1)).The material also showed a high relative density of 99.1%,indicating a compact and well-sintered microstructure,as confirmed by a three-point bending test.Furthermore,a high critical current density of 1.4 mA∙cm^(−2)was achieved in symmetric cell testing.Additionally,a Na_(3)V_(2)(PO_(4))_(3)||Zn-NZSP0.07||Na cell delivered an initial capacity of 103.9 mAh∙g^(−1)at 0.1 A∙g^(−1)and retained 73.4%of its capacity after 200 cycles.These results demonstrate that optimal heteroatom doping is crucial for enhancing the performance of NASICON.
