Density-functional calculations of the conversion of methane to methanol on platinum-decorated sheets of graphene oxide

作者：Wu Shiuan Yau; Lin Chien Hao; Ho Jia Jen^*

来源：Physical Chemistry Chemical Physics, 2015, 17(39): 26191-26197.

DOI：10.1039/c5cp03930d

By means of calculations based on density-functional theory (DFT), we have investigated the conversion of methane on two platinum atoms supported with a graphene-oxide sheet (Pt-2/GO). In our calculations, a CH4 molecule can be adsorbed around the Pt atoms of the Pt-2/GO sheet with adsorption energies within -0.11 to -0.53 eV; an elongated C-H bond indicates that Pt atoms on that sheet can activate the C-H bond of a CH4 molecule. The role of the GO sheet in the activation of CH4 was identified according to an analysis of the electronic density: the GO sheet induces the d-band of Pt atoms to generate several specific d(z2) state features above the Fermi level, which enabled the activation of the C-H bond of CH4 in generating an evident area of overlap with the hydrogen s orbital of the C-H bond. Upon a dioxygen molecule being added onto the Pt-2/GO sheet, this molecule can react with activated CH4 according to mechanisms of form 2CH(4) +O-2 ->([Pt2/GO]) 2CH(3)OH, and restore the original Pt-2/GO sheet.

• 出版日期2015