Single-crystal Nickel-rich layered oxides has been recognized as one of the promising cathodes for nextgeneration lithium batteries on account of their high capacity,while its practical application was hindered by str...Single-crystal Nickel-rich layered oxides has been recognized as one of the promising cathodes for nextgeneration lithium batteries on account of their high capacity,while its practical application was hindered by structural instability and slow Li^(+) transfer kinetics.Herein,a surface-to-bulk engineered single-crystal LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(Ni90) cathode,which features W-doped bulk and Li_(2)WO_(4) surface layer,was successfully achieved by a one-step high-valence W^(6+) modification.The as-obtained W-modified Ni90 delivers excellent cycling stability(89.8% capacity retention after 300 cycles at 0.5 C)and rate capability.The enhanced electrochemical performance was ascribed to the doped-W induced stabilized lattice oxygen,reduced Li^(+)/Ni^(2+) mixing and inhibited H2-H3 phase transition in the bulk,and Li_(2)WO_(4) layer generated stabilized cathode/electrolyte interface.In addition,the thinner LiF-rich cathode electrolyte interphase(CEI) on surface and smaller grain size for W-modified Ni90 benefit to its Li^(+) diffusion dynamics.The effect of high-valence W^(6+)on single-crystal Ni-rich cathode was firstly revealed in detail,which deepens the understanding of electrochemical behavior of Ni-rich cathode with high-valence cations modification,and provides clues for design of high-performance layered cathodes.展开更多
基金National Key Research and Development Program of China (2022YFB2502103)National Natural Science Foundation of China (22279107, 22309153)Fundamental Research Funds for the Central Universities (20720230039)。
文摘Single-crystal Nickel-rich layered oxides has been recognized as one of the promising cathodes for nextgeneration lithium batteries on account of their high capacity,while its practical application was hindered by structural instability and slow Li^(+) transfer kinetics.Herein,a surface-to-bulk engineered single-crystal LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(Ni90) cathode,which features W-doped bulk and Li_(2)WO_(4) surface layer,was successfully achieved by a one-step high-valence W^(6+) modification.The as-obtained W-modified Ni90 delivers excellent cycling stability(89.8% capacity retention after 300 cycles at 0.5 C)and rate capability.The enhanced electrochemical performance was ascribed to the doped-W induced stabilized lattice oxygen,reduced Li^(+)/Ni^(2+) mixing and inhibited H2-H3 phase transition in the bulk,and Li_(2)WO_(4) layer generated stabilized cathode/electrolyte interface.In addition,the thinner LiF-rich cathode electrolyte interphase(CEI) on surface and smaller grain size for W-modified Ni90 benefit to its Li^(+) diffusion dynamics.The effect of high-valence W^(6+)on single-crystal Ni-rich cathode was firstly revealed in detail,which deepens the understanding of electrochemical behavior of Ni-rich cathode with high-valence cations modification,and provides clues for design of high-performance layered cathodes.
