Interface optimization mechanism and quantitative analysis of hybrid graphite anode for fast-charging lithium-ion...

Due to the inherent characteristics of traditional graphite anode material, its lithium diffusion kinetic is significantly constrained, easily leading to a noticeable capacity degradation during rapid charge/discharge cycling. Although modifying the graphite by mixing the hard carbon can effectively enhance its fast-charging performance, yet the underlying mechanism of improvement effect and structure design of interface are still needed to further investigate. To address this research gap, hard carbon-coated graphite (HCCG) material has been designed and synthesized through simple interface engineering, which is aimed to explore and elucidate the optimization mechanisms on fast-charging performance from the graphite interface perspective. According to the electrochemical calculations, the HCCG anode exhibits significant enhancements. Specially, its reversible lithium content is increased by approximately 8 % at various states of charge, its exchange current density is tripled, and its Tafel slope is reduced to one-quarter of the original graphite. Therefore, the HCCG maintains an impressive 86.89 % capacity retention and a high capacity of 202.3 mAh g^-1 after 1450 cycles at ultrahigh rate of 5C. These improvements indicate a substantial reduction in electrode polarization during fast charging, which is ascribed to the abundant lithium intercalation pathways and accommodation space provided by the intimate hard carbon coating layer. Moreover, as a "buffer layer," hard carbon coating can accommodate considerable amount of lithium deposited on the graphite surface, effectively mitigating the capacity loss caused by lithium deposition and maintaining effective electrochemical contact without delamination. This comprehensive analysis of hard carbon coating illustrates the improvement mechanism of fast-charging performance, which can offer valuable insights into the dynamic and structural optimization of graphite anode interfaces.