Graphene coating-modified LiCoO2 films as high-performance cathode material in quasi-solid-state thin-film lithium batteries

LiCoO2 (LCO) films were successfully prepared using a radio frequency magnetron sputtering method, and the interface between the LCO cathode films and Li1.5Al0.5Ge1.5(PO4)3 (LAGP) solid electrolyte was modified by a graphene (G) buffer layer. The composition and morphology of the thin-film samples were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy. The LCO thin film annealed at 600 °C had excellent charge transport properties, respectively delivering initial charge and discharge specific capacities of 162.7 mAh·g−1 and 124.5 mAh·g−1 at 0.1C in a half-cell structure. Relaxation time distribution reconstruction impedance analysis and rate characteristic analysis of an LCO/G/LAGP/G/LCO symmetric cell demonstrated that the flexible graphene buffer layer effectively improved the contact impedance of the interface and structure stability of the active materials. After cycling for 1000 h at current densities of 0.02 mA·cm−2 and 0.5 mA·cm−2, the LCO/G/LAGP/G/LCO symmetric cell still maintained stable polarization voltages of 0.05 V and 0.7 V, respectively. In addition, an assembled LCO/G/LAGP/Li quasi-solid-state film lithium battery presented an initial discharge specific capacity of 109.53 mAh·g−1 at 0.1C, with a capacity retention rate of 71.86 % after 100 cycles.