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Breaking the energy density limit of Li NiO_(2):Li_(2)NiO_(3)or Li_(2)NiO_(2)?

Science China Materials 2022年第4期65卷 913-919页

作者： Yining Jia Yaokun Ye Jiahua Liu Shisheng Zheng Weicheng Lin Zhu Wang Shunning Li Feng Pan Jiaxin Zheng School of Advanced Materials Peking UniversityShenzhen Graduate SchoolShenzhen518055China Fujian science&technology innovation laboratory for energy devices of China(21C-LAB) Ningde352100China

The development of next-generation layered oxide cathodes for high-energy-density electrical vehicle Li-ion batteries(LIBs)is an urgent *** existing method is achieved by continuously increasing the Ni contents of Ni-based layered oxides,but it has been limited to LiNiO_(2).To break this limit and attain increased energy densities,a promising strategy,which involves the introduction of excess Li ions into transition metal(TM)layers to form Li-excess compounds Li_(2)MO_(3)(M is a TM cation),has attracted enormous interest ***,another strategy,which has been neglected in recent years,involves the insertion of an extra layer of Li ions between the TM and original Li layers to form Li_(2)MO_(2).In this study,typical reversible Li_(2)NiO_(3) and 1T-Li_(2)NiO_(2) were selected as two representative cathodes to break the limit of LiNiO_(2),thereby availing comprehensive comparison with LiNiO_(2) regarding their overall properties as cathodes from a theoretical ***,dissimilar to the Ni^(3+)/Ni^(4+)monoelectron cationic redox associated with LiNiO_(2),a polaronic anionic redox reaction occurs in Li_(2)NiO_(3),while a reversible Ni^(2+)/Ni^(4+)double-electron redox reaction accompanied by insulator-metal transition occurs in Li_(2)NiO_(2).Owing to this double-electron cationic activity,Li_(2)NiO_(2) exhibits absolute advantages over the other two materials(LiNiO_(2) and Li_(2)NiO_(3))as cathodes for LIBs in terms of the capacity,energy density,electronic conductivity,and thermal stability,thus rendering it the most promising candidate for next-generation layered oxide cathodes with high energy densities to break the limit of LiNiO_(2).

关键词： Li-ion battery Li_(2)NiO_(3)and Li_(2)NiO_(2) double-electron redox anionic redox theoretical perspective

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