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Methane to methanol conversion induced by thorium oxide through the CH3Th(O)H intermediate in solid argon.

Yu Gong¹, Lester Andrews, Virgil E Jackson

¹Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904-4319, USA.

Inorganic Chemistry

|September 26, 2012

Summary

Thorium oxide (ThO) facilitates methane to methanol conversion by forming a novel CH(3)Th(O)H intermediate. This reaction occurs at low temperatures and is confirmed through spectroscopic analysis and computational studies.

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Area of Science:

Inorganic Chemistry
Physical Chemistry
Computational Chemistry

Background:

Investigating the reactivity of small molecules and metal oxides is crucial for understanding catalytic processes.
Thorium oxide (ThO) is a potential catalyst, but its reaction mechanisms with hydrocarbons are not well-understood.
Low-temperature matrix isolation studies provide insights into reaction pathways and intermediate species.

Purpose of the Study:

To investigate the reaction between thorium oxide (ThO) and methane (CH(4)) in a solid argon matrix.
To identify and characterize any novel reaction intermediates formed during the process.
To elucidate the mechanism of methane to methanol conversion induced by ThO.

Main Methods:

Matrix isolation infrared spectroscopy at near 4 K.
Isotopic substitution (e.g., deuterium) to confirm vibrational assignments.
Electronic structure frequency calculations (CCSD(T)//B3LYP) to support experimental findings and determine reaction energetics.

Main Results:

Formation of a new intermediate, CH(3)Th(O)H, was observed upon UV irradiation of ThO and CH(4).
Spectroscopic evidence, including Th═O and Th-H stretching modes, confirmed the intermediate's structure.
Methanol formation correlated with the appearance of CH(3)Th(O)H, indicating its role in methane-to-methanol conversion.

Conclusions:

The reaction of ThO with CH(4) proceeds via the CH(3)Th(O)H intermediate, leading to methanol.
The initial reaction step is exothermic with a moderate energy barrier, while intermediate decomposition is endothermic.
Thorium atoms react with methanol without an activation energy, suggesting different reaction pathways.