To reduce surface contamination and increase battery life, MoO3 nanoparticles were coated with a high-voltage (5 V) LiNi0.5Mn1.5O4 cathode material by in-situ method during the high-temperature annealing process. To avoid charging by more than 5 V, we also developed a system based on anode-limited full-cell with a negative/positive electrode (N/P) ratio of 0.9. The pristine LiNi0.5Mn1.5O4 was initially prepared by high-energy ball-mill with a solid-state reaction, followed by a precipitation reaction with a molybdenum precursor for the MoO3 coating. The typical structural and electrochemical behaviors of the materials were clearly investigated and reported. The results revealed that a sample of 2 wt.% MoO3-coated LiNi0.5Mn1.5O4 electrode exhibited an optimal electrochemical activity, indicating that the MoO3 nanoparticle coating layers considerably enhanced the high-rate charge–discharge profiles and cycle life performance of LiNi0.5Mn1.5O4 with a negligible capacity decay. The 2 wt.% MoO3-coated LiNi0.5Mn1.5O4 electrode could achieve high specific discharge capacities of 131 and 124 mAh g−1 at the rates of 1 and 10 C, respectively. In particular, the 2 wt.% MoO3-coated LiNi0.5Mn1.5O4 electrode retained its specific capacity (87 mAh g−1) of 80.1% after 500 cycles at a rate of 10 C. The Li4Ti5O12/LiNi0.5Mn1.5O4 full cell based on the electrochemical-cell (EL-cell) configuration was successfully assembled and tested, exhibiting excellent cycling retention of 93.4% at a 1 C rate for 100 cycles. The results suggest that the MoO3 nano-coating layer could effectively reduce side reactions at the interface of the LiNi0.5Mn1.5O4 cathode and the electrolyte, thus improving the electrochemical performance of the battery system.

Morphology plays a vital role in controlling the volume variation in Si-based anode materials and enhances lithiumion battery performances. Here, we demonstrated advanced techniques that combine electrostatic self-assembly and spraydrying methods to form 3D spherical-like silicon/graphite (denoted "Si/G") composite anode materials. This spherical morphology alleviates issues relating to silicon volume changes that occur in high-rate lithium-ion batteries. Commercial graphite (G) flakes were initially mixed with silicon nanoparticles (ca. 50 nm) to form a bare-Si/G composite through electrostatic interaction; sphericallike composite particles were then obtained through single and double spray-drying processes, giving samples SD1-Si/G and SD2-Si/G, respectively. We examined the charge/discharge characteristics of the fabricated electrodes (CR2032-type coin cells) in the voltage range 0.02−1.5 V (vs Li/Li + ). The as-fabricated bare-Si/G, SD1-Si/G, and SD2-Si/G half-cells provided initial discharge specific capacities of 897, 866, and 1020 mA h g −1 , respectively. The SD2-Si/G half-cell shows better cycling stability at a high current rate of 400 mA g −1 than the SD1-Si/G and bare-Si/G half-cells due to effective inhibition of the volume change in the more stable spherical structure of the SD2-Si/G composite, as evidenced through in situ dilatometry. Thus, the spherical Si/G composite material produced through this simple spray-drying process had structural characteristics that could effectively resist silicon's high expansion rate, lower the production rate of broken silicon particles, and improve the electrochemical performance of the anode.

High-voltage spinel LiNi0.5Mn1.5O4 (LNMO) is a promising cathode material for next-generation lithium-ion batteries (LIBs), but its poor cycle performance has impeded its commercialization. In this study, we developed highly stable LNMO cathode materials having an octahedral morphology through a solid-state high-energy ball-mill–cum–spray-drying method. We also developed a novel strategy for modifying this cathode material with two kinds of carbon materials, thereby improving the electrochemical cycling performance. Introducing single-walled carbon nanotubes (SWCNTs) as a sub-carbon conductive additive during the slurry preparation process improved the conductivity of electrons between the particles of the cathode material. The LNMO electrode modified with the SWCNT sub-carbon additives exhibited an average Coulombic efficiency of 99.4% after 500 cycles at 1C, compared with 98.9% for the pristine LNMO-based electrode. Furthermore, we used a wet-chemical method to coat graphene oxide (GO) onto the post-sintered LNMO cathode material to act as a protective layer, preventing corrosion induced by HF in the electrolyte. The capacity retention of the GO-coated LNMO electrode after 500 cycles at 1C (91.8%) was higher than that of the pristine LNMO (52.5%). The corresponding dual-modification strategy, combining the SWCNTs and GO, provided LNMO cathode materials exhibiting superior rate performance and cyclability, with an average Coulombic efficiency of 99.3% and capacity retention of 92.9% after 500 cycles at 1C. Thus, the LNMO cathode materials prepared in this study possessed excellent electrochemical properties favoring their marketability, applicability, and competitiveness for application in high-voltage LIBs.

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