The development of all-solid-state lithium batteries(ASSLBs)depends on exploiting solid-state electrolytes(SSEs)with high ionic conductivity and electrochemical stability.Fluorination is generally considered to be an ...The development of all-solid-state lithium batteries(ASSLBs)depends on exploiting solid-state electrolytes(SSEs)with high ionic conductivity and electrochemical stability.Fluorination is generally considered to be an effective strategy to improve the ionic conductivity and electrochemical stability of inorganic SSEs.Here,we report the partial fluorination of the chlo rine sites in an antiperovskite,by which the orthorhombic Li_(2)OHCl was transformed into cubic Li_(2)OHCl_(0.9)F_(0.1),resulting in a fourfold increase in ionic conductivity at 30℃.The ab initio molecular dynamics simulations suggest that both the crystal symmetry and the anions electronegativity influence the diffusion of Li+in the antiperovskite structure.Besides,from the perspective of experiments and calculations,it is confirmed that fluorination is a feasible method to improve the electrochemical stability of antiperovskite SSEs.The LiFePO_(4)|Li cell based on Li_(2)OHCl_(0.9)F_(0.1) is also assembled and exhibits stable cycle performance,which indicates that fluorination of antiperovskite SSEs is an effective way to produce high-performance SSEs for practical application of ASSLBs.展开更多
基金supported by the National Key Research and Development Program of China(2020YFA0210701)the National Natural Science Foundation of China(22005134,12275119,U22A20439)+4 种基金the Shenzhen Science and Technology Program(RCBS20210609103647030)the Guangdong Basic and Applied Basic Research Foundation(2021A1515012403)the Shenzhen Science and Technology Program(KQTD20200820113047086)the Guangdong-Hong Kong-Macao Joint Laboratory for PhotonicThermal-Electrical Energy Materials and Devices(2019B121205001)the open research fund of Songshan Lake Materials Laboratory(2022SLABFK04)。
文摘The development of all-solid-state lithium batteries(ASSLBs)depends on exploiting solid-state electrolytes(SSEs)with high ionic conductivity and electrochemical stability.Fluorination is generally considered to be an effective strategy to improve the ionic conductivity and electrochemical stability of inorganic SSEs.Here,we report the partial fluorination of the chlo rine sites in an antiperovskite,by which the orthorhombic Li_(2)OHCl was transformed into cubic Li_(2)OHCl_(0.9)F_(0.1),resulting in a fourfold increase in ionic conductivity at 30℃.The ab initio molecular dynamics simulations suggest that both the crystal symmetry and the anions electronegativity influence the diffusion of Li+in the antiperovskite structure.Besides,from the perspective of experiments and calculations,it is confirmed that fluorination is a feasible method to improve the electrochemical stability of antiperovskite SSEs.The LiFePO_(4)|Li cell based on Li_(2)OHCl_(0.9)F_(0.1) is also assembled and exhibits stable cycle performance,which indicates that fluorination of antiperovskite SSEs is an effective way to produce high-performance SSEs for practical application of ASSLBs.
