The University of Southampton
University of Southampton Institutional Repository

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

Structural selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy
Structural selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy
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.
2520-1158
157-163
Dann, Ellie K.
6418a9ec-735e-472e-a8fe-985c330d1b81
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Blackmore, Rachel, Hazel
3584b852-92ac-4341-b303-786f67e41f77
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
Collier, Paul
5ef98081-0269-4b6f-8c29-8e50facf17db
Chutia, Arunabhiram
fe207bfe-0a7e-4369-8e62-bfa575399f83
Erden, Tugce Eralp
758531fc-bdd2-4122-bc1b-2e4438b1a282
Hardacre, Christopher
0715f59a-c82e-4844-a9f8-6a06fb36320f
Kroner, Anna
0494fd4b-dbaf-4b9d-b279-0edcdd3da27f
Nachtegaal, Maarten
37fbcbc5-08e8-4eda-9350-2b162693013f
Raj, Agnes
860391d6-4201-4664-b1c2-5c2b9ddee929
Rogers, Scott M.
81804d0d-1f08-4a12-b6c8-56d7d45a039b
Taylor, S.F. Rebecca
ee19946e-25ea-420b-80ac-8dfe226c843b
Thompson, Paul
b3ca30ec-7410-43fa-8bca-0874493435bf
Tierney, George F.
694c2d56-6765-4de2-a0dc-484e56e28bbd
Zeinalipour-Yazdi, Constantinos D.
a2fdde38-2e52-49c5-b1f2-247244999505
Goguet, Alexandre
4de6e217-9733-4d26-b041-ab996672d919
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Dann, Ellie K.
6418a9ec-735e-472e-a8fe-985c330d1b81
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Blackmore, Rachel, Hazel
3584b852-92ac-4341-b303-786f67e41f77
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
Collier, Paul
5ef98081-0269-4b6f-8c29-8e50facf17db
Chutia, Arunabhiram
fe207bfe-0a7e-4369-8e62-bfa575399f83
Erden, Tugce Eralp
758531fc-bdd2-4122-bc1b-2e4438b1a282
Hardacre, Christopher
0715f59a-c82e-4844-a9f8-6a06fb36320f
Kroner, Anna
0494fd4b-dbaf-4b9d-b279-0edcdd3da27f
Nachtegaal, Maarten
37fbcbc5-08e8-4eda-9350-2b162693013f
Raj, Agnes
860391d6-4201-4664-b1c2-5c2b9ddee929
Rogers, Scott M.
81804d0d-1f08-4a12-b6c8-56d7d45a039b
Taylor, S.F. Rebecca
ee19946e-25ea-420b-80ac-8dfe226c843b
Thompson, Paul
b3ca30ec-7410-43fa-8bca-0874493435bf
Tierney, George F.
694c2d56-6765-4de2-a0dc-484e56e28bbd
Zeinalipour-Yazdi, Constantinos D.
a2fdde38-2e52-49c5-b1f2-247244999505
Goguet, Alexandre
4de6e217-9733-4d26-b041-ab996672d919
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266

Dann, Ellie K., Gibson, Emma K., Blackmore, Rachel, Hazel, 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, 157-163. (doi:10.1038/s41929-018-0213-3).

Record type: Article

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.

Text
Dann_E_NH3-SCO_Main manuscript_Nov2018_incl.AUTHORS_V3 - Accepted Manuscript
Restricted to Repository staff only until 10 June 2019.
Request a copy

More information

Accepted/In Press date: 10 December 2018
e-pub ahead of print date: 28 January 2019

Identifiers

Local EPrints ID: 428164
URI: https://eprints.soton.ac.uk/id/eprint/428164
ISSN: 2520-1158
PURE UUID: af1c992d-56f4-4e16-823a-9fa731527419
ORCID for Peter P. Wells: ORCID iD orcid.org/0000-0002-0859-9172

Catalogue record

Date deposited: 13 Feb 2019 17:30
Last modified: 16 Apr 2019 00:34

Export record

Altmetrics

Contributors

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

University divisions

Download statistics

Downloads from ePrints over the past year. Other digital versions may also be available to download e.g. from the publisher's website.

View more statistics

Atom RSS 1.0 RSS 2.0

Contact ePrints Soton: eprints@soton.ac.uk

ePrints Soton supports OAI 2.0 with a base URL of https://eprints.soton.ac.uk/cgi/oai2

This repository has been built using EPrints software, developed at the University of Southampton, but available to everyone to use.

We use cookies to ensure that we give you the best experience on our website. If you continue without changing your settings, we will assume that you are happy to receive cookies on the University of Southampton website.

×