Although graphite materials with desirable comprehensive properties dominate the anode market of commercial lithium-ion batteries (LIBs), their low capacity during fast charging precludes further commercialization. In the present work, natural graphite (G) is reported not only to suffer from low capacity during fast charging, but also from charge failure after many charging cycles. Using different characterization techniques, severe graphite exfoliation, and continuously increasing solid electrolyte interphase (SEI) are demonstrated as reasons for the failure of G samples. An ultrathin artificial SEI is proposed, addressing these problems effectively and ensuring extremely stable operation of the graphite anode, with a capacity retention of ≈97.5% after 400 cycles at 1 C. Such an artificial SEI modification strategy provides a universal approach to tailoring and designing better anode materials for next-generation LIBs with high energy densities.

• Klíčová slova
• artificial solid electrolyte interphase (SEI), graphite anodes, graphite exfoliation,
• Publikační typ
• časopisecké články MeSH

Natural graphite, with its lower production cost, higher capacity, and superior electrical conductivity than artificial graphite, currently accounts for approximately 40% of the global lithium-ion battery anode market. However, the inadequate compatibility of natural graphite with commercial carbonate ester electrolytes leads to irreversible capacity loss, reduce coulombic efficiency, and rapid capacity decline during cycling. Applying an oxygen-deficient titanium dioxide (TiO2-x) protective layer to natural graphite anodes has been noted as a successful method for improving their structural integrity and cycling stability; however, the fragile solid-electrolyte interphase (SEI) limits their fast-charging capability. In this study, nitrogen atoms are strategically incorporated into the TiO2-x surface structures, creating a lychee-like primary interphase that regulated the interfacial electrochemistry and facilitated the development of a LiF-dominated SEI. The robust LiF-dominated SEI, as examined through ex situ X-ray photoelectron spectroscopy analysis and kinetic evaluations, successfully mitigates interfacial side reactions and enhances bulk charge transfer. Consequently, the modified natural graphite anodes exhibit improved capacities at higher current densities, delivering a stable reversible capacity of 388.9 mAh g-1 after 200 cycles at a rate of 5 C.

• Klíčová slova
• LiF‐dominated SEI, fast‐charging anode, lychee‐like primary interphase, natural graphite,
• Publikační typ
• časopisecké články MeSH