Stewart, C. et al. (2018) Unraveling the H2 promotional effect on the Palladium catalysed CO oxidation using a combination of temporally and spatially resolved investigations. ACS Catalysis, 8(9), pp. 8255-8262. (doi: 10.1021/acscatal.8b01509) (PMID:30221029) (PMCID:PMC6135604)
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Abstract
The promotional effect of H2 on the oxidation of CO is of topical interest and there is debate over whether this promotion is due to either thermal or chemical effects. As yet there is no definitive consensus in the literature. Combining spatially resolved mass spectrometry and X-ray absorption spectroscopy (XAS) we observe a specific environment of the active catalyst during CO oxidation, having the same specific local coordination of the Pd in both the absence and presence of H2. In combination with Temporal Analysis of Products (TAP), performed under isothermal conditions, a mechanistic insight into the promotional effect of H2 was found, providing clear evidence of non-thermal effects in the hydrogen promoted of oxidation of carbon monoxide. We have identified that H2 promotes the Langmuir Hinshelwood mechanism and we propose this is linked to the increased interaction of O with the Pd surface in the presence of H2. This combination of spatially resolved MS and XAS and TAP studies has provided previously unobserved insights into the nature of this promotional effect.
| Item Type: | Articles |
|---|---|
| Additional Information: | Funding Acknowledgements: RSC for assistance via a Researcher Mobility Grant and DEL (NI) for funding of the studentship for C.Stewart. The UK Catalysis Hub is thanked for funding (EPSRC UK grant EP/K014714/1). The Diamond Light Source are thanked for awarding the beamtime (Experiment number SP11747-1). Y-C Wang and S.J. Haigh acknowledge funding from the Chinese Scholarship Council (CSC) and European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (ERC-2016-STG-EvoluTEM-715502) and EPSRC grant EP/P009050/1. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Gibson, Dr Emma |
| Authors: | Stewart, C., Gibson, E. K., Morgan, K., Cibin, G., Dent, A., Hardacre, C., Kontdratenko, E., Kontdratenko, V., McManus, C., Rogers, S., Stere, C., Chansai, S., Wang, Y., Haigh, S., Wells, P., and Goguet, A. |
| College/School: | College of Science and Engineering > School of Chemistry |
| Journal Name: | ACS Catalysis |
| Publisher: | American Chemical Society |
| ISSN: | 2155-5435 |
| ISSN (Online): | 2155-5435 |
| Published Online: | 26 July 2018 |
| Copyright Holders: | Copyright © 2018 American Chemical Society |
| First Published: | First published in ACS Catalysis 8(9): 8255-8262 |
| Publisher Policy: | Reproduced under a Creative Commons License |
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