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

Ellie Dann, Emma Gibson, Rachel Blackmore, Richard Catlow, Paul Collier, Arunabhiram Chutia, Tugce Eralp Erden, Christopher Hardacre, Anna Kroner, Maarten Nachtegaal, Agnes Raj, Scott Rogers, Rebecca Taylor, Paul Thompson, George Tierney, Constantinos Zeinalipour-Yazdi, Alexandre Goguet, Peter Wells

Research output: Contribution to journalArticle

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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 PdNxspecies, and clarify the selectivity-directing structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N2.
Original languageEnglish
Pages (from-to)157–163
JournalNature Catalysis
Volume2
Early online date28 Jan 2019
DOIs
Publication statusPublished - 01 Feb 2019

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Catalytic oxidation
Nanoparticles
Spectrum Analysis
Catalyst selectivity
Spectroscopy
X ray absorption fine structure spectroscopy
Metal Nanoparticles
Vehicle Emissions
Reducing Agents
Catalyst supports
Density functional theory
Mass spectrometry
Mass Spectrometry
Nitrogen
X-Rays
Infrared radiation
Temperature

Cite this

Dann, Ellie ; Gibson, Emma ; Blackmore, Rachel ; Catlow, Richard ; Collier, Paul ; Chutia, Arunabhiram ; Eralp Erden, Tugce ; Hardacre, Christopher ; Kroner, Anna ; Nachtegaal, Maarten ; Raj, Agnes ; Rogers, Scott ; Taylor, Rebecca ; Thompson, Paul ; Tierney, George ; Zeinalipour-Yazdi, Constantinos ; Goguet, Alexandre ; Wells, Peter. / Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy. In: Nature Catalysis. 2019 ; Vol. 2. pp. 157–163.
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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 PdNxspecies, and clarify the selectivity-directing structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N2.",
author = "Ellie Dann and Emma Gibson and Rachel Blackmore and Richard Catlow and Paul Collier and Arunabhiram Chutia and {Eralp Erden}, Tugce and Christopher Hardacre and Anna Kroner and Maarten Nachtegaal and Agnes Raj and Scott Rogers and Rebecca Taylor and Paul Thompson and George Tierney and Constantinos Zeinalipour-Yazdi and Alexandre Goguet and Peter Wells",
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Dann, E, Gibson, E, Blackmore, R, Catlow, R, Collier, P, Chutia, A, Eralp Erden, T, Hardacre, C, Kroner, A, Nachtegaal, M, Raj, A, Rogers, S, Taylor, R, Thompson, P, Tierney, G, Zeinalipour-Yazdi, C, Goguet, A & Wells, P 2019, 'Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy', Nature Catalysis, vol. 2, pp. 157–163. https://doi.org/10.1038/s41929-018-0213-3

Structure Selectivity of Supported Pd nanoparticles for Catalytic NH3 Oxidation resolved using combined Operando Spectroscopy. / Dann, Ellie; Gibson, Emma; Blackmore, Rachel; Catlow, Richard; Collier, Paul; Chutia, Arunabhiram ; Eralp Erden, Tugce; Hardacre, Christopher; Kroner, Anna; Nachtegaal, Maarten; Raj, Agnes; Rogers, Scott; Taylor, Rebecca; Thompson, Paul; Tierney, George; Zeinalipour-Yazdi, Constantinos ; Goguet, Alexandre; Wells, Peter.

In: Nature Catalysis, Vol. 2, 01.02.2019, p. 157–163.

Research output: Contribution to journalArticle

TY - JOUR

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

AU - Dann, Ellie

AU - Gibson, Emma

AU - Blackmore, Rachel

AU - Catlow, Richard

AU - Collier, Paul

AU - Chutia, Arunabhiram

AU - Eralp Erden, Tugce

AU - Hardacre, Christopher

AU - Kroner, Anna

AU - Nachtegaal, Maarten

AU - Raj, Agnes

AU - Rogers, Scott

AU - Taylor, Rebecca

AU - Thompson, Paul

AU - Tierney, George

AU - Zeinalipour-Yazdi, Constantinos

AU - Goguet, Alexandre

AU - Wells, Peter

PY - 2019/2/1

Y1 - 2019/2/1

N2 - 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 PdNxspecies, and clarify the selectivity-directing structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N2.

AB - 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 PdNxspecies, and clarify the selectivity-directing structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N2.

U2 - 10.1038/s41929-018-0213-3

DO - 10.1038/s41929-018-0213-3

M3 - Article

VL - 2

SP - 157

EP - 163

JO - Nature Catalysis

JF - Nature Catalysis

SN - 2520-1158

ER -