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Towards the operational window for nitridic and carbidic palladium nanoparticles for directed catalysis

Towards the operational window for nitridic and carbidic palladium nanoparticles for directed catalysis
Towards the operational window for nitridic and carbidic palladium nanoparticles for directed catalysis
The reactions under which interstitial structures of Pd form are profoundly important and prevalent in catalysis; the formation and stability of Pd hydride structures are well understood, however, interstitial structures of the carbide and nitride are relatively under explored. This work reports a systematic study of the formation and stability of PdCx and PdNx at elevated temperatures and different atmospheres using in situ Pd L3 edge XANES spectroscopy. These studies were further complemented by the application of 14N MAS-NMR experiments and computational DFT investigations. The experiments confirmed that PdCx was significantly more stable than PdNx; 14N MAS-NMR provided direct confirmation on the formation of the nitride, however, the XANES studies evidenced very limited stability under the conditions employed. Moreover, the results suggest that the formation of the nitride imparts some structural changes that are not entirely reversible under the conditions used in these experiments. This work provides important insights into the stability of interstitial structures of Pd and the conditions in which they could be employed for directed catalytic processes.
DFT modelling, heterogeneous catalysts, nanoparticles, operando spectroscopy, palladium nitride
1867-3880
Costley-wood, Lucy G.
d71f6b73-e732-4919-9728-c40997386312
Mohammed, Khaled
1c3c5641-4d0a-4c4d-bb26-fe733b8dbf63
Carravetta, Marina
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Decarolis, Donato
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Goguet, Alexandre
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Kordatos, Apostolos
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Vakili, Reza
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Manyar, Haresh
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Mcpake, Erin
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Skylaris, Chris-Kriton
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Thompson, Paul
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Gibson, Emma K.
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Wells, Peter
bc4fdc2d-a490-41bf-86cc-400edecf2266
Costley-wood, Lucy G.
d71f6b73-e732-4919-9728-c40997386312
Mohammed, Khaled
1c3c5641-4d0a-4c4d-bb26-fe733b8dbf63
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Decarolis, Donato
aa002823-ac92-4afe-aa03-83562110dd3c
Goguet, Alexandre
4de6e217-9733-4d26-b041-ab996672d919
Kordatos, Apostolos
f95fcb92-92b1-4ec8-991a-de7609845493
Vakili, Reza
7e37d2f5-ccc7-4530-9b77-898141c35ab2
Manyar, Haresh
aad00507-84ce-431c-ac0b-85dc1992ad6b
Mcpake, Erin
da60243b-e9f0-487c-a2a4-f783a003472a
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Thompson, Paul
1d328b8b-7c39-46d3-9fab-44933e256ef3
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Wells, Peter
bc4fdc2d-a490-41bf-86cc-400edecf2266

Costley-wood, Lucy G., Mohammed, Khaled, Carravetta, Marina, Decarolis, Donato, Goguet, Alexandre, Kordatos, Apostolos, Vakili, Reza, Manyar, Haresh, Mcpake, Erin, Skylaris, Chris-Kriton, Thompson, Paul, Gibson, Emma K. and Wells, Peter (2023) Towards the operational window for nitridic and carbidic palladium nanoparticles for directed catalysis. ChemCatChem, 15 (21), [e202300870]. (doi:10.1002/cctc.202300870).

Record type: Article

Abstract

The reactions under which interstitial structures of Pd form are profoundly important and prevalent in catalysis; the formation and stability of Pd hydride structures are well understood, however, interstitial structures of the carbide and nitride are relatively under explored. This work reports a systematic study of the formation and stability of PdCx and PdNx at elevated temperatures and different atmospheres using in situ Pd L3 edge XANES spectroscopy. These studies were further complemented by the application of 14N MAS-NMR experiments and computational DFT investigations. The experiments confirmed that PdCx was significantly more stable than PdNx; 14N MAS-NMR provided direct confirmation on the formation of the nitride, however, the XANES studies evidenced very limited stability under the conditions employed. Moreover, the results suggest that the formation of the nitride imparts some structural changes that are not entirely reversible under the conditions used in these experiments. This work provides important insights into the stability of interstitial structures of Pd and the conditions in which they could be employed for directed catalytic processes.

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ChemCatChem - 2023 - Costley-Wood - Version of Record
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Accepted/In Press date: 1 September 2023
e-pub ahead of print date: 7 September 2023
Published date: 8 November 2023
Additional Information: Funding Information: XMaS is a UK national research facility supported by EPSRC. We are grateful to all the beamline team staff on BM28 for their support, particularly Paul Thompson. Beamtime award number CH6009. Financial support is acknowledged to the EPSRC (EP/V000691/1) and the UKCP consortium (EP/P022030/1) for access to the ARCHER2 supercomputer. Also to the Materials and Molecular Modelling Hub (EP/T022213/1) and for access to the Young supercomputer, and the University of Southampton for access to the Iridis5 supercomputer. Donato Decarolis and Peter Wells acknowledges funded received through the UK Catalysis Hub and the UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026815/1, EP/R026939/1, EP/R026645/1 or EP/R027129/1. Funding Information: . XMaS is a UK national research facility supported by EPSRC. We are grateful to all the beamline team staff on BM28 for their support, particularly Paul Thompson. Beamtime award number CH6009. Financial support is acknowledged to the EPSRC (EP/V000691/1) and the UKCP consortium (EP/P022030/1) for access to the ARCHER2 supercomputer. Also to the Materials and Molecular Modelling Hub (EP/T022213/1) and for access to the Young supercomputer, and the University of Southampton for access to the Iridis5 supercomputer. Donato Decarolis and Peter Wells acknowledges funded received through the UK Catalysis Hub and the UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026815/1, EP/R026939/1, EP/R026645/1 or EP/R027129/1 Publisher Copyright: © 2023 The Authors. ChemCatChem published by Wiley-VCH GmbH.
Keywords: DFT modelling, heterogeneous catalysts, nanoparticles, operando spectroscopy, palladium nitride

Identifiers

Local EPrints ID: 481945
URI: http://eprints.soton.ac.uk/id/eprint/481945
DOI: doi:10.1002/cctc.202300870
ISSN: 1867-3880
PURE UUID: 29f1c3a8-c912-4d9d-b037-0b8952a7190f
ORCID for Khaled Mohammed: ORCID iD orcid.org/0000-0002-9538-0936
ORCID for Marina Carravetta: ORCID iD orcid.org/0000-0002-6296-2104
ORCID for Apostolos Kordatos: ORCID iD orcid.org/0000-0002-0183-8142
ORCID for Chris-Kriton Skylaris: ORCID iD orcid.org/0000-0003-0258-3433
ORCID for Peter Wells: ORCID iD orcid.org/0000-0002-0859-9172

Catalogue record

Date deposited: 13 Sep 2023 17:21
Last modified: 18 Mar 2024 04:02

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Contributors

Author: Lucy G. Costley-wood
Author: Khaled Mohammed ORCID iD
Author: Marina Carravetta ORCID iD
Author: Donato Decarolis
Author: Alexandre Goguet
Author: Apostolos Kordatos ORCID iD
Author: Reza Vakili
Author: Haresh Manyar
Author: Erin Mcpake
Author: Chris-Kriton Skylaris ORCID iD
Author: Paul Thompson
Author: Emma K. Gibson
Author: Peter Wells ORCID iD

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