Lithium-rich layered cathode material(LLM)can meet the requirement of power lithium-ion energy storage devices due to the great energy density.However,the de/intercalation of Li+will cause the irreversible loss of lat...Lithium-rich layered cathode material(LLM)can meet the requirement of power lithium-ion energy storage devices due to the great energy density.However,the de/intercalation of Li+will cause the irreversible loss of lattice oxygen and trigger transition metal(TM)ions migrate to Li+vacancies,resulting in capacity decay.Here we brought Ti4+in substitution of TM ions in Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2),which could stabilize structure and expand the layer spacing of LLM.Moreover,optimized Ti-substitution can regulate the anions and cations of LLM,enhance the interaction with lattice oxygen,increase Ni^(3+) and Co^(3+),and improve Mn^(4+) coordination,improving reversibility of oxygen redox activation,maintaining the stable framework and facilitating the Li^(+) diffusion.Furthermore,we found 5%Ti-substitution sample delivered a high discharge capacity of 244.2 mAh/g at 50 mA/g,an improved cycling stability to 87.3%after 100 cycles and enhanced rate performance.Thereby Ti-substitution gives a new pathway to achieve high reversible cycle retention for LLMs.展开更多
Lithium-rich layered oxides(LrLOs) deliver extremely high specific capacities and are considered to be promising candidates for electric vehicle and smart grid applications. However, the application of LrLOs needs fur...Lithium-rich layered oxides(LrLOs) deliver extremely high specific capacities and are considered to be promising candidates for electric vehicle and smart grid applications. However, the application of LrLOs needs further understanding of the structural complexity and dynamic evolution of monoclinic and rhombohedral phases, in order to overcome the issues including voltage decay, poor rate capability, initial irreversible capacity loss and etc. The development of aberration correction for the transmission electron microscope and concurrent progress in electron spectroscopy, have fueled rapid progress in the understanding of the mechanism of such issues. New techniques based on the transmission electron microscope are first surveyed, and the applications of these techniques for the study of the structure, migration of transition metal, and the activation of oxygen of LrLOs are then explored in detail, with a particular focus on the mechanism of voltage decay.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51972258,22109186).
文摘Lithium-rich layered cathode material(LLM)can meet the requirement of power lithium-ion energy storage devices due to the great energy density.However,the de/intercalation of Li+will cause the irreversible loss of lattice oxygen and trigger transition metal(TM)ions migrate to Li+vacancies,resulting in capacity decay.Here we brought Ti4+in substitution of TM ions in Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2),which could stabilize structure and expand the layer spacing of LLM.Moreover,optimized Ti-substitution can regulate the anions and cations of LLM,enhance the interaction with lattice oxygen,increase Ni^(3+) and Co^(3+),and improve Mn^(4+) coordination,improving reversibility of oxygen redox activation,maintaining the stable framework and facilitating the Li^(+) diffusion.Furthermore,we found 5%Ti-substitution sample delivered a high discharge capacity of 244.2 mAh/g at 50 mA/g,an improved cycling stability to 87.3%after 100 cycles and enhanced rate performance.Thereby Ti-substitution gives a new pathway to achieve high reversible cycle retention for LLMs.
基金finically supported by the National Key Research and Development Program of China (Grant No. 2016YFB0100100)Strategic Priority Research Program of Chinese Academy of Sciences (CAS, Grant No. XDA09010101)Ningbo Key Science and Technology Projects "Industrial Application Development of Graphene" (Grant No. 2014S10008)
文摘Lithium-rich layered oxides(LrLOs) deliver extremely high specific capacities and are considered to be promising candidates for electric vehicle and smart grid applications. However, the application of LrLOs needs further understanding of the structural complexity and dynamic evolution of monoclinic and rhombohedral phases, in order to overcome the issues including voltage decay, poor rate capability, initial irreversible capacity loss and etc. The development of aberration correction for the transmission electron microscope and concurrent progress in electron spectroscopy, have fueled rapid progress in the understanding of the mechanism of such issues. New techniques based on the transmission electron microscope are first surveyed, and the applications of these techniques for the study of the structure, migration of transition metal, and the activation of oxygen of LrLOs are then explored in detail, with a particular focus on the mechanism of voltage decay.