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Probing the role of a non-thermal plasma (NTP) in the hybrid NTP-catalytic oxidation of CH4

DOI: 10.1002/anie.201703550 DOI Help

Authors: Emma K. Gibson (University College London; UK Catalysis Hub) , C. Elena Stere (University of Manchester) , Bronagh Curran-mcateer (Queen's University of Belfast) , Wilm Jones (UK Catalysis; Cardiff Catalysis Institute, Cardiff University) , Giannantonio Cibin (Diamond Light Source) , Diego Gianolio (Diamond Light Source) , Alexandre Goguet (Queen's University of Belfast) , Peter Wells (UK Catalysis Hub; Diamond Light Source; University of Southampton) , C. Richard A. Catlow (UK Catalysis Hub; University College London) , Paul Collier (Johnson Matthey Technology Centre) , Peter Hinde (Johnson Matthey Technology Centre) , Christopher Hardacre (University of Manchester)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: June 2017
Diamond Proposal Number(s): 12986 , 10306

Abstract: Three recurring hypothesis are often used to explain the effect of non-thermal plasma (NTP) on NTP-catalytic hybrid reactions, namely, modification or heating of the catalyst or the ability of plasma produced species to open up new reaction pathways. By directly monitoring the catalyst by X-ray absorption fine structure (XAFS) coupled with end of pipe mass spectrometry the NTP assisted CH4 oxidation over Pd/Al2O3 was investigated. This in situ study has shown that the catalyst did not undergo any significant structural changes under NTP conditions. However, the NTP did lead to the Pd nanoparticle temperature increasing but 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) via electron impact reactions is proposed.

Journal Keywords: non-thermal plasma; EXAFS spectroscopy; oxidation; Heterogeneous Catalysis; Methane

Subject Areas: Chemistry

Instruments: B18-Core EXAFS