Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy

Dann, Ellie K. and Gibson, Emma K. and Blackmore, Rachel H. and Catlow, Richard A. and Collier, Paul and Chutia, Arunabhiram and Erden, Tugce Eralp and Hardacre, Christopher and Kroner, Anna and Nachtegaal, Maarten and Raj, Agnes and Rogers, Scott M. and Taylor, S.F. Rebecca and Thompson, Paul and Tierney, George F. and Constantinos D., Zeinalipour-Yazdi and Coguet, Alexandre and Wells, Peter P. (2019) Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy. Nature Catalysis, 2 . pp. 157-163. ISSN 2520-1158

Full content URL: https://doi.org/10.1038/s41929-018-0213-3

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Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy
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Abstract

The selective catalytic oxidation of NH3 to N2 (NH3-SCO) presents a promising solution for abatement of unused NH3-based reductants from diesel exhaust after treatment systems. 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 is found by operando X-ray absorption Fine Structure (XAFS) spectroscopy, diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) and on-line mass spectrometry. Nitrogen insertion into the metallic Pd nanoparticle structure at low temperatures (< 200°C) is 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 for combined operando spectroscopy and DFT calculations to characterise a previously unidentified PdNx catalyst, and clarify the selectivity directing structure of supported Pd catalysts for NH3-SCO.

Keywords:Pd nanoparticle, DFT, operando spectroscopy
Subjects:F Physical Sciences > F100 Chemistry
Divisions:College of Science > School of Chemistry
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ID Code:34854
Deposited On:18 Feb 2019 11:47

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