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[Display omitted] Benefiting from the extra contribution of O redox, Co-free Li-rich layered oxides (LRNMO) can satisfy the requirement of high specific capacities. However, during the high-voltage charging process, lattice oxygen being oxidized to O− or O 2 leads to a gradual transition of the structure from layered to spinel phase, capacity and voltage decline, hindering the practical application of LRNMO in the lithium-ion battery. Here, a surface modification strategy of Li 1.2 Ni 0.32 Mn 0.48 O 2-δ doped with Ta5+ ions is proposed, in which the Ta5+ ions occupy the lithium sites of the lattice structure on the surface layer of LRNMO and form a Ta 2 O 5 coating layer. The modified electrode exhibits excellent rate performance and cycling stability, with 94.9% and 85.5% capacity retention rate and voltage retention rate, respectively, after 200 cycles at 1C. Moreover, the initial coulomb efficiency and ionic conductivity of the modified electrode are also apparently enhanced. Simultaneously, the decreased Li/Ni mixing degree of the modified electrode reflects the improvement of the structural stability. Therefore, the modification strategy through strong metal–oxygen bonding to integrate the surface structure to regulate the oxygen activity provides a new direction for the design of high energy density Co-free Li-rich cathode materials. [ABSTRACT FROM AUTHOR]

[Display omitted] Benefiting from the extra contribution of O redox, Co-free Li-rich layered oxides (LRNMO) can satisfy the requirement of high specific capacities. However, during the high-voltage charging process, lattice oxygen being oxidized to O− or O 2 leads to a gradual transition of the structure from layered to spinel phase, capacity and voltage decline, hindering the practical application of LRNMO in the lithium-ion battery. Here, a surface modification strategy of Li 1.2 Ni 0.32 Mn 0.48 O 2-δ doped with Ta5+ ions is proposed, in which the Ta5+ ions occupy the lithium sites of the lattice structure on the surface layer of LRNMO and form a Ta 2 O 5 coating layer. The modified electrode exhibits excellent rate performance and cycling stability, with 94.9% and 85.5% capacity retention rate and voltage retention rate, respectively, after 200 cycles at 1C. Moreover, the initial coulomb efficiency and ionic conductivity of the modified electrode are also apparently enhanced. Simultaneously, the decreased Li/Ni mixing degree of the modified electrode reflects the improvement of the structural stability. Therefore, the modification strategy through strong metal–oxygen bonding to integrate the surface structure to regulate the oxygen activity provides a new direction for the design of high energy density Co-free Li-rich cathode materials. [ABSTRACT FROM AUTHOR]

• Polypyrrole coating is utilized for polysulfides immobilization. • Lithium sulfide is wrapped inside cathode from exposure. • Activation barrier and polysulfides shuttle are greatly suppressed. • Electrochemical performances of as-prepared cells are promoted. The significantly-high theoretical energy density and eco-sustainability of lithium sulfur batteries (LSBs) arouses a rapid surge of interest in recent years. However, some key issues of cathode, for instance, the polysulfides confinement, low ion/electrons transfer and etc., hinder the practical utilization of LSBs. Herein, such issues could be carefully handled by using the conductive polypyrrole as polysulfides wrapper. The polypyrrole with pyrrole rings can efficiently confine polysulfides inside cathode for redox. Meanwhile, the conductive polypyrrole with delocalized π-electron cloud can facilitate electrons transfer. Besides, the addition of carbon nanotube (CNT) and oxidized graphene (GO) can enhance the conductivity of cathode material. As a result, the Li 2 S/CNT/GO/PPy cathode delivers a cycling capacity of 525 mAh g−1 with a low-capacity decay rate of 0.065 % cycle−1 after 400 cycles. Therefore, the lithium-sulfur battery with Li 2 S-based and PPy-wrapped cathode could reasonably be counted as a potential alternative of long-cycling Li-ion cells. [Display omitted] [ABSTRACT FROM AUTHOR]