Theoretical Study The Chemical Modification Andthe Build Of High-performance Catalyst About Two-dimensional Na Nomaterials

The two-dimensional material graphene, one planar sheet of sp²-bonded carbon atoms arranged in a hexagonal lattice, is attractive for a wide variety of research fields due to its unique optical, electrical, magnetic, and mechanical properties. Recently study showed that chemical doped have shown to be effective in modifying the intrinsic properties of graphene, including electronic and magnetic characteristics. Among various possible dopants（such as B, N, S, F, and P）, N-doping exhibits obvious advantages. Hexagonal boron nitride（h-BN） nanosheet, a structural analogue to graphene have higher thermal stability and chemical stability than graphene. But the pristine h-BN sheet is a wide-band gap（-6eV） semiconductors, which limit its applications. The study found that chemical modification can not only enhance the solubility of BN nanosheet, and can effectively tune the electric and magnetic properties of BN nanosheet, thus broaden its application to some extent.In this paper, we investigated the deposition of Pt₁3 nanoparticles on N-doped graphene, and the affect of electronic property of h-BN sheet for CHO modification.（1） We firstly investigated the structural and electronic properties of Pt₁3 nanoparticles on various nitrogen（N）-doped graphene and their interaction with O by density functional theory（DFT） calculations. The results revealed that the N-doping can greatly enhance the binding strength of Pt₁3 nanoparticles on the graphene surface, thus ensuring their high stability. Moreover, a certain amount of electrons are transferred from Pt₁3 to the substrate accompanied by a substantial downshift of the Pt₁3 d-band center, thus greatly weakening the interaction of O on these composites.（2） We performed density functional theory（DFT） calculations to study the adsorption of CHO radicals with different coverages on h-BN sheet. Particular attention is paid to explore the effects of CHO adsorption on the geometrical structures and electronic properties of h-BN sheet. The results indicate that the adsorption of a single CHO radical on pristine h-BN sheet is very weak with a negligible adsorption energy（-0.09eV）. In contrast, upon adsorption of more CHO radicals on h-BN sheet, these adsorbates prefer to adsorb in pairs on the B and the nearest N atoms from both sides of h-BN sheet. The coverage rate of CHO radicals is up to 40% with the adsorption energy of-0.29 eV. the CHO modification can tune the band gap of h-BN sheeet effectively, and further strengthen its conductivity.The results of this study indicate that N-doped graphenes not only stabilize the Pt clusters but also enhance their catalytic performance in the oxygen reduction reaction and can act as a catalyst for the oxygen reduction reaction hopefully. The chemical modification of CHO radical can effective reducing the band gap of h-BN sheet and provide a theoretical guidance and clues to broaden its applications.