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Atomically Defined Templates for Epitaxial Growth of Complex Oxide Thin Films

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Published on: December 4, 2014

Methane Chemisorption on Oxide-Supported Pt Single Atom.

Victor Fung¹, Guoxiang Hu², Franklin Feng Tao³

¹Department of Chemistry, University of California, Riverside, California, 92521, United States.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry

|July 18, 2019

Summary

The occupancy of the platinum d_z² orbital dictates methane chemisorption on oxide surfaces. This key factor enables strong methane adsorption on semiconducting oxides like TiO₂ but prevents it on metallic oxides.

Keywords:

density functional theory electronic structure metal oxides methane adsorption single atom

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Area of Science:

Surface Science
Computational Chemistry
Materials Science

Background:

Methane chemisorption on single-atom catalysts is crucial for various chemical processes.
Recent studies demonstrated methane chemisorption on rutile iridium dioxide (IrO₂) (110).
General requirements for methane chemisorption on single atoms supported by oxides remain unclear.

Purpose of the Study:

To elucidate the general requirements for methane chemisorption on single platinum atoms (Pt₁) supported by rutile-type oxides.
To identify the key electronic properties governing the interaction between Pt single atoms and oxide supports for methane adsorption.

Main Methods:

Utilized hybrid density functional theory (DFT) calculations.
Investigated methane adsorption on Pt₁ substitutionally doped on various rutile-type oxides (e.g., TiO₂, GeO₂, IrO₂, RuO₂).

Main Results:

The occupancy of the platinum d_z² orbital is identified as the critical factor for methane chemisorption.
Strong methane chemisorption occurs on semiconducting/wide-gap oxides (TiO₂, GeO₂) due to an empty Pt d_z² orbital accepting electron donation from methane's C-H bond.
Weak or no methane chemisorption occurs on metallic oxides (IrO₂, RuO₂) as the Pt d_z² orbital becomes more occupied due to mixing with oxide electronic states.

Conclusions:

The electronic interaction between the single Pt atom and the oxide support significantly influences methane adsorption.
Tuning the electronic properties of the oxide support can control the chemisorption capability of supported single Pt atoms for methane.