The spinel Mn-based cathodes with 3D Li+ diffusion channels, high voltage, and low-cost show promise for developing high-power lithium-ion batteries (LIBs). But the disproportionation and Jahn-Teller distortion lead to structural degeneration and capacity decay, especially at high working temperatures. Herein, considering the merits of single crystals and orientation of exposed crystal planes, single-crystal truncated octahedral LiMn2 O4 (TO-LMO) with exposed {111}, {100} and {110} facets is rationally designed, in which the mainly exposed {111} facets are truncated by a small portion of {100} and {110} facets. The Li-deficient intermediate phase is innovatively proposed to prepare the single-crystal TO-LMO. The synergistic effects of single crystals and the orientation of exposed crystal planes significantly reduce the disproportionation of Mn3+ ions and thereby improve their structural stability. Consequently, the cycling stability of the single-crystal TO-LMO is remarkably enhanced, obtaining outstanding capacity retention of 84.3% after 2000 cycles, much better than that of 61.2% for octahedral LiMn2 O4 . The feasibility of preparing single-crystal truncated octahedral LiNi0.5 Mn1.5 O4 with exposed {111}, {100}, and {110} facets via the Li-deficient intermediate phase is further demonstrated. These findings offer new insight into regulating the orientation of exposed crystal planes and improving the reversibility of Mn-based redox couples in LIBs. 

General Synthesis of Single-Crystal Spinel Cathodes with the Tailored Orientation of Exposed Crystal Planes for Advanced Lithium-Ion Batteries.

Spinel lithium manganese oxide, LiMn2O4 coated with V2O5 layer (labeled as LMO-VO) has been developed and its electrochemical performances as cathode material for lithium-ion batteries has been evaluated at high cut-off voltage (>4.5 V vs. Li/Li+) and compared with pristine LiMn2O4 (labeled as LMO). The crystal structure investigations show that LMO-VO has longer Li–O bond length for fast Li-ion diffusion kinetic process. The scanning electron microscopy results indicate that LMO-VO has finer particles and the V2O5 layer has been successfully coated on the LMO surface uniformly. The highly conductive V2O5 coating layer enhances the ionic conductivity of the LMO cathode, as evidenced by the significant drop of Rct value from the Nyquist plot. Under high operating voltage, the cell employed with coated LMO shows exceptional cycling performance in capacity retention and potential difference. After 300 cycles, the capacity retention per cycle has been boosted from 99.90% to 99.94% by adopting the V2O5 coating layer. In addition, surface coating with V2O5 stabilizes the potential difference at very minimal change for a longer period. This convincingly proves that the V2O5 coating layer not only protects against hydrofluoric acid (HF) attack and greatly restrains the increase of cell polarization at high voltage. 

Improved cycling stability of V
 2
 O
 5
 modified spinel LiMn
 2
 O
 4
 Cathode at High cut‐off voltage for lithium‐ion batteries

Recent progress in the fabrication of controlled structures and advanced materials has improved battery performance in terms of specific capacity, rate capability, and cycling stability. However, interfacial problems such as increased resistance and contact instability between the electrodes and solid/liquid electrolytes still put pressure on the controllable formation of structures and the improvement of performance as well as safety. Here, we first briefly introduce the deposition techniques in terms of working mechanism and experimental process, then illustrate the associated advantages/disadvantages of the surface engineering methods based on deposition techniques (physical vapor deposition and chemical reaction deposition) to the provision of reference for researchers selecting the appropriate approach. Second, we exemplify the Si/LiCoO2/LiPON/Li to demonstrate the main progress made in lithium-ion batteries, elaborating on the efforts in engineering the reactive surface utilizing the deposition techniques. Finally, general conclusions and prospects for future advanced thin film deposition techniques in the field of lithium-ion batteries are presented.

/pdf/thin-film-deposition-techniques-in-surface-engineering-1oreu7j8.pdf

Thin Film Deposition Techniques in Surface Engineering Strategies for Advanced Lithium-Ion Batteries


 Lithium cobalt oxide (LiCoO2, LCO) thin-film cathodes are usually prepared with slow deposition rates by sputtering techniques. Atmospheric plasma spraying (APS) is a possible technology for the rapid deposition method replacing sputter deposition to fabricate all-solid-state lithium batteries. This study employed the APS device to rapidly deposit LCO thick films as cathodes with deposition rates exceeding 5,400 nm/min. The results show that the LCO cathodes have presented a specific capacity of 120 mAh/g after being annealed and assembled in a gel polymer electrolyte lithium battery. Furthermore, the LCO cathodes also demonstrated a high areal capacity of 5.65 mAh/cm2, one of the best areal capacity performances. Therefore, APS technology offers a highly competitive approach to commercializing energy storage products.

LiCoO2 Battery Electrode Fabricated by High Deposition-Rate Atmospheric Plasma Spraying for Lithium Battery

Abstract LiMn2O4 has the advantages of low cost and no pollution, and is widely regarded as a large-scale lithium battery cathode material. However, the capacity decays rapidly, which seriously affects the application of LiMn2O4 cathode materials. Therefore, improving the cycling performance of LiMn2O4 is the focus of current research. LiMn2O4 precursors were prepared by chemical precipitation and the precursors were coated to prepare LiMn2O4/TiO2 composites. X-ray diffraction and scanning electron microscopy showed that LiMn2O4 had been successfully combined with TiO2. Electrode charge–discharge and electrochemical impedance tests showed that LiMn2O4/TiO2 had the best cycle performance at high rates. The initial discharge capacities of LiMn2O4/TiO2 reached 106.4 mAh·g−1 at 0.2 C. After 100 cycles, the 2 C capacity retention rates was 76.3 %, compared to only 66.5 % for pristine LiMn2O4. The improved electrochemical performance was attributed to the nanoscale oxides hindering the reaction between the electrolyte and the electrode, which effectively improved the stability of the material during high current charge and discharge.

Enhanced high-rate cycling performance of LiMn2O4 cathode materials by coating nano-TiO2

Nanostructure distortion improvement of Al doped spinel LiMn2O4 films deposited by RF magnetron sputtering for flexible high-voltage lithium ion batteries

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Nanostructure distortion improvement of Al doped spinel LiMn2O4 films deposited by RF magnetron sputtering for flexible high-voltage lithium ion batteries