Probing the Role of a Non‐Thermal Plasma (NTP) in the Hybrid NTP Catalytic Oxidation of Methane

Three recurring hypotheses are often used to explain the effect of non‐thermal plasmas (NTPs) on NTP catalytic hybrid reactions; namely, modification or heating of the catalyst or creation of new reaction pathways by plasma‐produced species. NTP‐assisted methane (CH4) oxidation over Pd/Al2O3 was inv...

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Published in:Angewandte Chemie International Edition 2017-08, Vol.56 (32), p.9351-9355
Main Authors: Gibson, Emma K, Stere, Cristina E, Curran‐McAteer, Bronagh, Jones, Wilm, Cibin, Giannantonio, Gianolio, Diego, Goguet, Alexandre, Wells, Peter P., Catlow, C. Richard A., Collier, Paul, Hinde, Peter, Hardacre, Christopher
Format: Article
Language:English
Subjects:
Aluminum oxide
Catalysts
Catalytic oxidation
Communication
Communications
Electron impact
EXAFS spectroscopy
Fine structure
heterogeneous catalysis
Mass spectrometry
Mass spectroscopy
Methane
Nanoparticles
non-thermal plasma
Oxidation
Pipes
Plasmas (physics)
Temperature effects
Thermal plasmas
Ultrastructure
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Summary:Three recurring hypotheses are often used to explain the effect of non‐thermal plasmas (NTPs) on NTP catalytic hybrid reactions; namely, modification or heating of the catalyst or creation of new reaction pathways by plasma‐produced species. NTP‐assisted methane (CH4) oxidation over Pd/Al2O3 was investigated by direct monitoring of the X‐ray absorption fine structure of the catalyst, coupled with end‐of‐pipe mass spectrometry. This in situ study revealed that the catalyst did not undergo any significant structural changes under NTP conditions. However, the NTP did lead to an increase in the temperature of the Pd nanoparticles; although this temperature rise was insufficient to activate the thermal CH4 oxidation reaction. The contribution of a lower activation barrier alternative reaction pathway involving the formation of CH3(g) from electron impact reactions is proposed. Methane combustion was undertaken using a hybrid non‐thermal plasma palladium‐based catalyst system without heating of the catalyst bed. No significant structural changes were found in the catalyst by in situ X‐ray absorption spectroscopy. Plasma heating of the palladium nanoparticles did not introduce sufficient energy to activate methane oxidation, thus an alternative reaction pathway is proposed.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201703550