Preparation of High-Strength and High-Rigidity Carbon Layer on Si/C Material Surface Using Solid–Liquid Coating Method

The application of silicon-carbon (Si/C) composite materials in lithium-ion batteries faces problems regarding volume expansion and surface defects. Although coating is a popular modification scheme in the market, the influence of carbon layer quality on the electrochemical performance of Si/C still needs to be studied. By comparing the carbon layers produced by solid-phase and liquid-phase coating methods, an innovative solid-liquid coating technology was proposed to prepare high-strength and high-stiffness carbon layers, and the effects of different coating processes on the physical, mechanical, and electrochemical properties of the materials were systematically studied. Through physical properties and electrochemical testing, it was found that the solid-liquid coating method (Si/C@Pitch+RGFQ) can form a carbon layer with the least defects and the highest density. Compared with solid-phase coating and liquid-phase coating, its specific surface area (SSA) and carbon increment are the lowest, and the surface carbon content and oxygen content are significantly reduced after solid-liquid coating. Mechanical performance tests show that the Young's modulus of the carbon layer prepared by this method reaches 30.3 GPa, demonstrating excellent structural strength and elastic deformation ability. The first coulombic efficiency (ICE) of Si/C@Pitch+RGFQ reached 88.17%, the interface impedance (23.2 Ω) was the lowest, and the lithium-ion diffusion coefficient was significantly improved. At a rate of 0.1 C to 2 C, the capacity retention rate is excellent. After one hundred and a half-cell cycles, the remaining capacity is 1420.5 mAh/g, and the capacity retention rate reaches 92.4%. The full-cell test further proves that the material has a capacity retention rate of 82.3% and 81.3% after 1000 cycles at room temperature and high temperature (45 °C), respectively. At the same time, it has good rate performance and high-/low-temperature performance, demonstrating good commercial application potential. The research results provide a key basis for the optimized preparation of the surface carbon layer of Si/C composite materials and promote the practical application of high-performance silicon-based negative electrode materials.