▎ 摘　　要

The electronic structures of graphene nanoflakes (GNEs) exposed to an organo-silane precursor [tetramethylsilane, TMS, Si(CH3)(4)] were studied using electron field emission (EFE), Raman spectroscopy, X-ray absorption near-edge structure (XANES), X-ray photoelectron spectroscopy (XPS), X-ray emission spectroscopy (XES), and first-principles calculation. The results of XANES, XPS, and Raman spectroscopy indicate that the silyl radical strong covalent bonds were formed in GNFs, which induced local structural relaxations and enhanced sp(3) hybridization. Comparison of calculated electronic structure, XANES, and XES spectra of Si-treated GNFs suggests that the Si atom substitutes one 3-fold coordinated C atom in a given graphene layer and relaxes outward to form sp(3) bonding with another C atom in the adjacent graphene layer. The EFE measurements show an increase in the tum-on electric field with the increase of the Si content, which suggests an enhancement of the nonmetallic sp(3) bonding.