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

Dann, Ellie K., Gibson, Emma K., Blackmore, Rachel H., Catlow, C. Richard A., Collier, Paul, Chutia, Arunabhiram, Erden, Tugce Eralp, Hardacre, Christopher, Kroner, Anna, Nachtegaal, Maarten, Raj, Agnes, Rogers, Scott M., Taylor, S. F. Rebecca, Thompson, Paul, Tierney, George F., Zeinalipour-Yazdi, Constantinos D., Goguet, Alexandre and Wells, Peter P. 2019. Structural selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy. Nature Catalysis 2 , pp. 157-163. 10.1038/s41929-018-0213-3

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Abstract

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: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Advanced Research Computing @ Cardiff (ARCCA)
Cardiff Catalysis Institute (CCI)
ISSN: 2520-1158
Date of First Compliant Deposit: 11 February 2019
Date of Acceptance: 10 December 2018
Last Modified: 18 Oct 2019 00:28
URI: http://orca-mwe.cf.ac.uk/id/eprint/119425

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