Density-functional calculations of the conversion of methane to methanol on platinum-decorated sheets of graphene oxide
文献信息
Shiuan-Yau Wu, Chien-Hao Lin, Jia-Jen Ho
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 (Pt2/GO). In our calculations, a CH4 molecule can be adsorbed around the Pt atoms of the Pt2/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 dz2 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 Pt2/GO sheet, this molecule can react with activated CH4 according to mechanisms of form , and restore the original Pt2/GO sheet.
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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