Application of N-Doped Carbon–Silicon Oxycarbide Based on POSS Synthesis in Lithium-Ion Batteries

Abstract

Si/C materials have attracted much attention as anode materials for lithium-ion batteries. Here, nitrogen-doped silica carbon composites with a carbon-coated structure were synthesized using poly(1-vinylimidazole) in the presence of octavinyl-silsesquioxane followed by annealing and magnesium thermal reduction processes of the polymer precursor (PPVIm). Benefiting from the moderate Si–O–C bonds, the prepared NSiOC possesses a high first discharge capacity of 1862.3 mAh·g–1 at 0.2 A·g–1 and an initial Coulombic efficiency of 70.0% at 30 °C. When the temperature rises to 60 °C, the first discharge and charge specific capacities of the synthesized anode material at 0.2 A·g–1 increase to 2103.0 and 1528.7 mAh·g–1 with an ultralong lifespan of more than 1000 cycles. Moreover, the results show that the degradation of performance during the initial phase of cycles can be ascribed to the formation of an SEI layer and insufficient electrolyte penetration. The battery maintains a steady state (nearly 600 consecutive cycles) for a long time afterward as the activation of the anode material increases, attributed to the low expansion coefficient originating from the porous structure of the carbon capping layer and silicon oxide. In addition, the electrochemical attenuation process of the electrode material with a unique inorganic silica skeleton and exceptional electrochemical performance was also investigated for the assistance of future design in high-performance electrode materials.