High-Quality Epitaxial N Doped Graphene on SiC with Tunable Interfacial Interactions via Electron/Ion Bridges for Stable Lithium-Ion Storage

Tailoring the interfacial interaction in SiC-based anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage. In this paper, atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene (NG) on SiC (NG@SiC). This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction, making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration. Both density functional theory (DFT) analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds, enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation. As a proof-of-concept study, this well-designed NG@SiC anode shows good reversible capacity (1197.5 mAh g(−1) after 200 cycles at 0.1 A g(−1)) and cycling durability with 76.6% capacity retention at 447.8 mAh g(−1) after 1000 cycles at 10.0 A g(−1). As expected, the lithium-ion full cell (LiFePO(4)/C//NG@SiC) shows superior rate capability and cycling stability. This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01175-6.