Structure selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy

Dann, E. K. et al. (2019) Structure selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy. Nature Catalysis, 2(2), pp. 157-163. (doi: 10.1038/s41929-018-0213-3)

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The selective catalytic oxidation of NH3 to N2 presents a promising solution for the abatement of unused NH3-based reductants from diesel exhaust after treatment. Supported Pd nanoparticle catalysts show selectivity to N2 rather than NOx, which is investigated in this work. The link between Pd nanoparticle structure and surface reactivity was found using operando X-ray absorption fine structure spectroscopy, diffuse reflectance infrared Fourier-transformed spectroscopy and on-line mass spectrometry. Nitrogen insertion into the metallic Pd nanoparticle structure at low temperatures (<200 °C) was found to be responsible for high N2 selectivity, whereas the unfavourable formation of NO is linked to adsorbed nitrates, which form at the surface of bulk PdO nanoparticles at high temperatures (>280 °C). Our work demonstrates the ability of combined operando spectroscopy and density functional theory calculations to characterize a previously unidentified PdNx species, and clarify the selectivity-directing structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N2.

Item Type:Articles
Glasgow Author(s) Enlighten ID:Gibson, Dr Emma
Authors: Dann, E. K., Gibson, E. K., Blackmore, R. H., Catlow, C. R. A., Collier, P., Chutia, A., Erden, T. E., Hardacre, C., Kroner, A., Nachtegaal, M., Raj, A., Rogers, S. M., Taylor, S.F. R., Thompson, P., Tierney, G. F., Zeinalipour-Yazdi, C. D., Goguet, A., and Wells, P. P.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Nature Catalysis
Publisher:Nature Research
ISSN (Online):2520-1158
Published Online:28 January 2019
Copyright Holders:Copyright © 2019 Springer Nature Publishing AG
First Published:First published in Nature Catalysis 2(2): 157-163
Publisher Policy:Reproduced in accordance with the publisher copyright policy

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
652891Towards closing the chlorine cycle in large-scale chemical manufacturing processes (UK Catalysis hub)David LennonEngineering and Physical Sciences Research Council (EPSRC)EP/K014854/1CHEM - CHEMISTRY