Li-rich Mn-based oxides(LRMOs)hold great promise as next-generation cathode materials for high-energy Li-ion batteries because of their low cost and high capacity.Nevertheless,the practical application of LRMOs is imp...Li-rich Mn-based oxides(LRMOs)hold great promise as next-generation cathode materials for high-energy Li-ion batteries because of their low cost and high capacity.Nevertheless,the practical application of LRMOs is impeded by their low initial Coulombic efficiency and rapid voltage decay.Herein,a V-doped layered-spinel coherent layer is constructed on the surface of a Co-free LRMO through a simple treatment with NH_(4)VO_(3).The layered-spinel coherent layer with 3D ion channels enhanced Li+diffusion efficiency,mitigates surface-inter-face reactions and suppresses irreversible oxygen release.Notably,V-doping significantly reduces the Bader charge of oxygen atoms,thereby impeding excessive oxidation of oxygen ions and further enhancing the stability of O-redox.The modified LRMO exhibites a remarkable initial Coulombic efficiency of 91.6%,signifi-cantly surpassing that of the original LRMO(74.4%).Furthermore,the treated sample showes an impressive capacity retention rate of 91.9%after 200 cycles,accompanied by a voltage decay of merely 0.47 mV per cycle.The proposed treatment approach is straightforward and significantly improves the initial Coulombic efficiency,voltage stability,and capacity stability of LRMO cathode materials,thus holding considerable promise for the development of high-energy Li-ion batteries.展开更多
基金Natural Science Research(Department of Education)Project of Higher Education Institutions in Guangdong Province(Grant No.2018KQNCX063)Applied Basic Research Fund of Guangdong Province(Grant No.2024B1515020071)+1 种基金National Natural Science Foundation of China(Grant Nos.52371217 and 52150410411)Guangdong Provincial Science and Technology Plan Project(Grant No.2023A0505020009)。
文摘Li-rich Mn-based oxides(LRMOs)hold great promise as next-generation cathode materials for high-energy Li-ion batteries because of their low cost and high capacity.Nevertheless,the practical application of LRMOs is impeded by their low initial Coulombic efficiency and rapid voltage decay.Herein,a V-doped layered-spinel coherent layer is constructed on the surface of a Co-free LRMO through a simple treatment with NH_(4)VO_(3).The layered-spinel coherent layer with 3D ion channels enhanced Li+diffusion efficiency,mitigates surface-inter-face reactions and suppresses irreversible oxygen release.Notably,V-doping significantly reduces the Bader charge of oxygen atoms,thereby impeding excessive oxidation of oxygen ions and further enhancing the stability of O-redox.The modified LRMO exhibites a remarkable initial Coulombic efficiency of 91.6%,signifi-cantly surpassing that of the original LRMO(74.4%).Furthermore,the treated sample showes an impressive capacity retention rate of 91.9%after 200 cycles,accompanied by a voltage decay of merely 0.47 mV per cycle.The proposed treatment approach is straightforward and significantly improves the initial Coulombic efficiency,voltage stability,and capacity stability of LRMO cathode materials,thus holding considerable promise for the development of high-energy Li-ion batteries.
