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

Ellie K.  Dann; Emma K Gibson; Rachel H. Blackmore; C Richard A Catlow; Paul Collier; Arunabhiram Chutia; Tugce Eralp  Erden; Christopher Hardacre; Anna  Kroner; Maarten Nachtegaal; Agnes  Raj; Scott M. Rogers; S F Rebecca Taylor; Paul Thompson; George F. Tierney; Constantinos D. Zeinalipour-Yazdi; Alexandre Goguet; Peter P.  Wells

doi:10.1038/s41929-018-0213-3

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

Ellie K. Dann, Emma K Gibson, Rachel H. Blackmore, C Richard A Catlow, Paul Collier, Arunabhiram Chutia, Tugce Eralp Erden, Christopher Hardacre, Anna Kroner, Maarten Nachtegaal, Agnes Raj, Scott M. Rogers, S F Rebecca Taylor, Paul Thompson, George F. Tierney, Constantinos D. Zeinalipour-Yazdi, Alexandre Goguet, Peter P. Wells

Queen's University Belfast

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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.

Original language	English
Journal	Nature Catalysis
Early online date	28 Jan 2019
DOIs	https://doi.org/10.1038/s41929-018-0213-3
Publication status	Published - 2019

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Photon Science Institute
Dalton Nuclear Institute

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Dann_E_NH3-SCO_Main manuscript_Nov2018_incl.AUTHORS_V3Accepted author manuscript, 1 MB

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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., & Wells, P. P. (2019). Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy. Nature Catalysis. https://doi.org/10.1038/s41929-018-0213-3

@article{f8792a8ef9dd47f391660ac875268b6c,

title = "Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy",

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. ",

author = "Dann, {Ellie K.} and Gibson, {Emma K} and Blackmore, {Rachel H.} and Catlow, {C Richard A} and Paul Collier and Arunabhiram Chutia and Erden, {Tugce Eralp} and Christopher Hardacre and Anna Kroner and Maarten Nachtegaal and Agnes Raj and Rogers, {Scott M.} and Taylor, {S F Rebecca} and Paul Thompson and Tierney, {George F.} and Zeinalipour-Yazdi, {Constantinos D.} and Alexandre Goguet and Wells, {Peter P.}",

year = "2019",

doi = "10.1038/s41929-018-0213-3",

language = "English",

journal = "Nature Catalysis",

issn = "2520-1158",

publisher = "Springer Nature",

}

Dann, EK, Gibson, EK, Blackmore, RH, Catlow, CRA, Collier, P, Chutia, A, Erden, TE, Hardacre, C, Kroner, A, Nachtegaal, M, Raj, A, Rogers, SM, Taylor, SFR, Thompson, P, Tierney, GF, Zeinalipour-Yazdi, CD, Goguet, A & Wells, PP 2019, 'Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy', Nature Catalysis. https://doi.org/10.1038/s41929-018-0213-3

TY - JOUR

T1 - Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy

AU - Dann, Ellie K.

AU - Gibson, Emma K

AU - Blackmore, Rachel H.

AU - Catlow, C Richard A

AU - Collier, Paul

AU - Chutia, Arunabhiram

AU - Erden, Tugce Eralp

AU - Hardacre, Christopher

AU - Kroner, Anna

AU - Nachtegaal, Maarten

AU - Raj, Agnes

AU - Rogers, Scott M.

AU - Taylor, S F Rebecca

AU - Thompson, Paul

AU - Tierney, George F.

AU - Zeinalipour-Yazdi, Constantinos D.

AU - Goguet, Alexandre

AU - Wells, Peter P.

PY - 2019

Y1 - 2019

N2 - 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.

AB - 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.

U2 - 10.1038/s41929-018-0213-3

DO - 10.1038/s41929-018-0213-3

M3 - Article

SN - 2520-1158

JO - Nature Catalysis

JF - Nature Catalysis

ER -

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

Abstract

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