The garnet Li₇La₃Zr₂O₁₂ (LLZO) has been widely investigated because of its high conductivity, wide electrochemical window, and chemical stability with regards to lithium metal. However, the usual preparation process of LLZO requires high-temperature sintering for a long time and a lot of mother powder to compensate for lithium evaporation. In this study submicron Li_6.6La₃Zr_1.6Nb_0.4O₁₂ (LLZNO) powder―which has a stable cubic phase and high sintering activity―was prepared using the conventional solid-state reaction and the attrition milling process, and Li stoichiometric LLZNO ceramics were obtained by sintering this powder―which is difficult to control under high sintering temperatures and when sintered for a long time―at a relatively low temperature or for a short amount of time. The particle-size distribution, phase structure, microstructure, distribution of elements, total ionic conductivity, relative density, and activation energy of the submicron LLZNO powder and the LLZNO ceramics were tested and analyzed using laser diffraction particle-size analyzer (LD), X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), Electrochemical Impedance Spectroscopy (EIS), and the Archimedean method. The total ionic conductivity of samples sintered at 1200 °C for 30 min was 5.09 × 10⁻⁴ S·cm⁻¹, the activation energy was 0.311 eV, and the relative density was 87.3%. When the samples were sintered at 1150 °C for 60 min the total ionic conductivity was 3.49 × 10⁻⁴ S·cm⁻¹, the activation energy was 0.316 eV, and the relative density was 90.4%. At the same time, quasi-solid-state batteries were assembled with LiMn₂O₄ as the positive electrode and submicron LLZNO powder as the solid-state electrolyte. After 50 cycles, the discharge specific capacity was 105.5 mAh/g and the columbic efficiency was above 95%.

Nickel-rich layered LiNi_1−x−yCo_xMn_yO₂ (LiMO₂) is widely investigated as a promising cathode material for advanced lithium-ion batteries used in electric vehicles, and a much higher energy density in higher cut-off voltage is emergent for long driving range. However, during extensive cycling when charged to higher voltage, the battery exhibits severe capacity fading and obvious structural collapse, which leads to poor cycle stability. Herein, Sn-doping and in situ formed Li₂SnO₃ nano-coating layer co-modified spherical-like LiNi_0.5Co_0.2Mn_0.3O₂ samples were successfully prepared using a facile molten salt method and demonstrated excellent cyclic properties and high-rate capabilities. The transition metal site was expected to be substituted by Sn in this study. The original crystal structures of the layered materials were influenced by Sn-doping. Sn not only entered into the crystal lattice of LiNi_0.5Co_0.2Mn_0.3O₂, but also formed Li⁺-conductive Li₂SnO₃ on the surface. Sn-doping and Li₂SnO₃ coating layer co-modification are helpful to optimize the ratio of Ni²⁺ and Ni³⁺, and to improve the conductivity of the cathode. The reversible capacity and rate capability of the cathode are improved by Sn-modification. The 3 mol% Sn-modified LiNi_0.5Co_0.2Mn_0.3O₂ sample maintained the reversible capacity of 146.8 mAh g⁻¹ at 5C, corresponding to 75.8% of its low-rate capacity (0.1C, 193.7mAh g⁻¹) and kept the reversible capacity of 157.3 mAh g⁻¹ with 88.4% capacity retention after 100 charge and discharge cycles at 1C rate between 2.7 and 4.6 V, showing the improved electrochemical property.

Li-rich layered oxide cathode materials have become one of the most promising cathode materials for high specific energy lithium-ion batteries owning to its high theoretical specific capacity, low cost, high operating voltage and environmental friendliness. Yet they suffer from severe capacity and voltage attenuation during prolong cycling, which blocks their commercial application. To clarify these causes, we synthesize Li_1.5Mn_0.55Ni_0.4Co_0.05O_2.5 (Li_1.2Mn_0.44Ni_0.32Co_0.04O₂) with high-nickel-content cathode material by a solid-sate complexation method, and it manifests a lot slower capacity and voltage attenuation during prolong cycling compared to Li_1.5Mn_0.66Ni_0.17Co_0.17O_2.5 (Li_1.2Mn_0.54Ni_0.13Co_0.13O₂) and Li_1.5Mn_0.65Ni_0.25Co_0.1O_2.5 (Li_1.2Mn_0.52Ni_0.2Co_0.08O₂) cathode materials. The capacity retention at 1 C after 100 cycles reaches to 87.5% and the voltage attenuation after 100 cycles is only 0.460 V. Combining X-ray diffraction (XRD), scanning electron microscope (SEM), and transmission electron microscopy (TEM), it indicates that increasing the nickel content not only stabilizes the structure but also alleviates the attenuation of capacity and voltage. Therefore, it provides a new idea for designing of Li-rich layered oxide cathode materials that suppress voltage and capacity attenuation.

Lithium-rich layered oxide is one of the most promising candidates for the next-generation cathode materials of high-energy-density lithium ion batteries because of its high discharge capacity. However, it has the disadvantages of uneven composition, voltage decay, and poor rate capacity, which are closely related to the preparation method. Here, 0.5Li₂MnO₃·0.5LiMn_0.8Ni_0.1Co_0.1O₂ was successfully prepared by sol–gel and oxalate co-precipitation methods. A systematic analysis of the materials shows that the 0.5Li₂MnO₃·0.5LiMn_0.8Ni_0.1Co_0.1O₂ prepared by the oxalic acid co-precipitation method had the most stable layered structure and the best electrochemical performance. The initial discharge specific capacity was 261.6 mAh·g⁻¹ at 0.05 C, and the discharge specific capacity was 138 mAh·g⁻¹ at 5 C. The voltage decay was only 210 mV, and the capacity retention was 94.2% after 100 cycles at 1 C. The suppression of voltage decay can be attributed to the high nickel content and uniform element distribution. In addition, tightly packed porous spheres help to reduce lithium ion diffusion energy and improve the stability of the layered structure, thereby improving cycle stability and rate capacity. This conclusion provides a reference for designing high-energy-density lithium-ion batteries.

The chlorine (Cl) and bromine (Br) co-doped lithium nickel manganese cobalt oxide (LiNi_1/3Co_1/3Mn_1/3O₂) was successfully synthesized by the molten salt method. The synthesized LiNi_1/3Co_1/3Mn_1/3O₂ compound demonstrates spherical morphology, which is formed by aggregated spherical-like or polygon primary particles. Halogen substitution would contribute to the growth of the primary particles. The LiNi_1/3Co_1/3Mn_1/3O₂ compound has the typical hexagonal layered structure, and no impurity phase is detected. The surface oxidation state of the compound is improved after Cl and Br substitution. Moreover, the Cl and Br co-doped LiNi_1/3Co_1/3Mn_1/3O₂ compound exhibits both improved rate capacity and cycle stability at a high voltage (4.6 V) compared with the pristine LiNi_1/3Co_1/3Mn_1/3O₂. The initial discharge capacities of Cl and Br co-doped LiNi_1/3Co_1/3Mn_1/3O₂ are 208.9 mAh g⁻¹, 200.6 mAh g⁻¹, 188.2 mAh g⁻¹, 173.3 mAh g⁻¹, and 157.1 mAh g⁻¹ at the corresponding rates of 0.1C, 0.2C, 0.5C, 1C, and 3C respectively. The capacity retention at 1C after 50 cycles is increased from 81.1% to 93.2% by co-doping. The better contact between the electroactive particles of the electrode and the smaller resistance enhance the electric conductivity of the Cl and Br co-doped LiNi_1/3Co_1/3Mn_1/3O₂ cathode. The synthesized LiNi_1/3Co_1/3Mn_1/3O₂ is a promising cathode material for a high-power and large-capacity lithium-ion battery.