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

Shiuan Yau Wu; Chien Hao Lin; Jia Jen Ho

doi:10.1039/c5cp03930d

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

Shiuan Yau Wu, Chien Hao Lin, Jia Jen Ho^*

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

27 Citations (Scopus)

Abstract

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 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 Pt₂/GO sheet, this molecule can react with activated CH₄ according to mechanisms of form, and restore the original Pt₂/GO sheet.

Original language	English
Pages (from-to)	26191-26197
Number of pages	7
Journal	Physical Chemistry Chemical Physics
Volume	17
Issue number	39
DOIs	https://doi.org/10.1039/c5cp03930d
Publication status	Published - 2015 Sept 4

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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

abstract = "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.",

author = "Wu, {Shiuan Yau} and Lin, {Chien Hao} and Ho, {Jia Jen}",

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T1 - Density-functional calculations of the conversion of methane to methanol on platinum-decorated sheets of graphene oxide

AU - Wu, Shiuan Yau

AU - Lin, Chien Hao

AU - Ho, Jia Jen

N1 - Publisher Copyright: This journal is © the Owner Societies.

PY - 2015/9/4

Y1 - 2015/9/4

N2 - 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.

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

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