Engineering lithium-ion battery cathodes for high-voltage applications using electromagnetic excitation

Microwave radiation (MWR), a type of electromagnetic excitation source, reduces the synthesis temperature and processing time for chemical reactions compared to traditional synthesis methods. Recently, we demonstrated that MWR can engineer ceramics with different crystal phases compared to traditional methods [Journal of Materials Chemistry A5, 35 (2017)]. In this study, we further apply the MWR-assisted technique to improve the electrochemical performance of LiCoO2 cathodes by engineering TiO2 and ZrO2 ceramic coatings. Electrochemical tests suggest that the TiO2 coating improves the rate capability of the LiCoO2 electrode. Both TiO2 and ZrO2 coatings improve the high-voltage (4.5 V) cycling stability of LiCoO2. The capacity remaining is improved from 52.8 to 84.4% and 81.9% by the TiO2 coating and the ZrO2 coating, respectively, after 40 cycles. We compare these results with existing studies that apply traditional methods to engineer TiO2/ZrO2 on LiCoO2, and find that the MWR-assisted method shows better performance improvement. X-ray photoelectron spectroscopy measurements suggest that the improved cycling stability arises from the formation of metal fluorides that protect the electrode from side reactions with electrolytes. This mechanism is further supported by the reduced Co dissolution from TiO2/ZrO2-coated LiCoO2 electrode after cycling. This study provides a new toolbox facilitating the integration of many delicate, low melting point materials like polymers into battery electrodes.