Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure

Atta ul Haq; Fiorenza Fanelli; Leonidas Bekris; Alex Martinez Martin; Steve Lee; Hessan Khalid; Cristian D. Savaniu; Kalliopi  Kousi; Ian S.  Metcalfe; John T. S. Irvine; Paul Maguire; Evangelos I. Papaioannou; Davide Mariotti

doi:10.1002/advs.202402235

Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure

Atta ul Haq, Fiorenza Fanelli, Leonidas Bekris, Alex Martinez Martin, Steve Lee, Hessan Khalid, Cristian D. Savaniu, Kalliopi Kousi, Ian S. Metcalfe, John T. S. Irvine, Paul Maguire, Evangelos I. Papaioannou, Davide Mariotti

Design, Manufacturing And Engineering Management

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Abstract

Exsolution of metal nanoparticles (NPs) on perovskite oxides has been demonstrated as a reliable strategy for producing catalyst-support systems. Conventional exsolution requires high temperatures for long periods of time, limiting the selection of support materials. We report plasma direct exsolution at room temperature and atmospheric pressure of Ni NPs from a model A-site deficient perovskite oxide (La_0.43Ca_0.37Ni_0.06Ti_0.94O_2.955). Plasma exsolution is carried out within minutes (up to 15 min) using a dielectric barrier discharge configuration both with He-only gas as well as with He/H₂ gas mixtures, yielding small NPs (< 30 nm diameter). To prove the practical utility of exsolved NPs, we have carried out various experiments aimed at assessing their catalytic performance for methanation from synthesis gas, CO and CH₄ oxidation. We successfully demonstrated low-temperature and atmospheric pressure plasma exsolution and suggest that this approach could contribute to the practical deployment of exsolution-based stable catalyst systems.

Original language	English
Article number	2402235
Number of pages	15
Journal	Advanced Science
Volume	11
Issue number	34
Early online date	4 Jul 2024
DOIs	https://doi.org/10.1002/advs.202402235
Publication status	Published - 11 Sept 2024

Funding

This work has been supported by EPSRC through the UK Catalysis Hub (EP/R027129/1) and the Emergent Nanomaterials-Critical Mass Initiative (EP/R023638/1, EP/R023921/1, EP/R023522/1, EP/R008841/1) as well as the Royal Society (IES\R2\212049). F.F. gratefully acknowledges support from the National Research Council of Italy (2020 STM program). I.S.M. acknowledges funding from the Royal Academy of Engineering through a Chair in Emerging Technologies Award entitled “Engineering Chemical Reactor Technologies for a Low-Carbon Energy Future” (Grant CiET1819\2\57). KK acknowledges funding from the Henry Royce Institute (EP/X527257/1).

Keywords

nanoparticles
perovskite oxides
catalyst-support systems
exsolution
dielectric barrier discharge

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10.1002/advs.202402235Licence: CC BY 4.0

Haq-etal-AS-2024-Dielectric-barrier-plasma-discharge-exsolution-of-nanoparticlesFinal published version, 6.49 MBLicence: CC BY 4.0

Cite this

Haq, A. U., Fanelli, F., Bekris, L., Martin, A. M., Lee, S., Khalid, H., Savaniu, C. D., Kousi, K., Metcalfe, I. S., Irvine, J. T. S., Maguire, P., Papaioannou, E. I., & Mariotti, D. (2024). Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure. Advanced Science, 11(34), Article 2402235. https://doi.org/10.1002/advs.202402235

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title = "Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure",

abstract = "Exsolution of metal nanoparticles (NPs) on perovskite oxides has been demonstrated as a reliable strategy for producing catalyst-support systems. Conventional exsolution requires high temperatures for long periods of time, limiting the selection of support materials. We report plasma direct exsolution at room temperature and atmospheric pressure of Ni NPs from a model A-site deficient perovskite oxide (La0.43Ca0.37Ni0.06Ti0.94O2.955). Plasma exsolution is carried out within minutes (up to 15 min) using a dielectric barrier discharge configuration both with He-only gas as well as with He/H2 gas mixtures, yielding small NPs (< 30 nm diameter). To prove the practical utility of exsolved NPs, we have carried out various experiments aimed at assessing their catalytic performance for methanation from synthesis gas, CO and CH4 oxidation. We successfully demonstrated low-temperature and atmospheric pressure plasma exsolution and suggest that this approach could contribute to the practical deployment of exsolution-based stable catalyst systems.",

keywords = "nanoparticles, perovskite oxides, catalyst-support systems, exsolution, dielectric barrier discharge",

author = "Haq, {Atta ul} and Fiorenza Fanelli and Leonidas Bekris and Martin, {Alex Martinez} and Steve Lee and Hessan Khalid and Savaniu, {Cristian D.} and Kalliopi Kousi and Metcalfe, {Ian S.} and Irvine, {John T. S.} and Paul Maguire and Papaioannou, {Evangelos I.} and Davide Mariotti",

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AU - Haq, Atta ul

AU - Fanelli, Fiorenza

AU - Bekris, Leonidas

AU - Martin, Alex Martinez

AU - Lee, Steve

AU - Khalid, Hessan

AU - Savaniu, Cristian D.

AU - Kousi, Kalliopi

AU - Metcalfe, Ian S.

AU - Irvine, John T. S.

AU - Maguire, Paul

AU - Papaioannou, Evangelos I.

AU - Mariotti, Davide

PY - 2024/9/11

Y1 - 2024/9/11

N2 - Exsolution of metal nanoparticles (NPs) on perovskite oxides has been demonstrated as a reliable strategy for producing catalyst-support systems. Conventional exsolution requires high temperatures for long periods of time, limiting the selection of support materials. We report plasma direct exsolution at room temperature and atmospheric pressure of Ni NPs from a model A-site deficient perovskite oxide (La0.43Ca0.37Ni0.06Ti0.94O2.955). Plasma exsolution is carried out within minutes (up to 15 min) using a dielectric barrier discharge configuration both with He-only gas as well as with He/H2 gas mixtures, yielding small NPs (< 30 nm diameter). To prove the practical utility of exsolved NPs, we have carried out various experiments aimed at assessing their catalytic performance for methanation from synthesis gas, CO and CH4 oxidation. We successfully demonstrated low-temperature and atmospheric pressure plasma exsolution and suggest that this approach could contribute to the practical deployment of exsolution-based stable catalyst systems.

AB - Exsolution of metal nanoparticles (NPs) on perovskite oxides has been demonstrated as a reliable strategy for producing catalyst-support systems. Conventional exsolution requires high temperatures for long periods of time, limiting the selection of support materials. We report plasma direct exsolution at room temperature and atmospheric pressure of Ni NPs from a model A-site deficient perovskite oxide (La0.43Ca0.37Ni0.06Ti0.94O2.955). Plasma exsolution is carried out within minutes (up to 15 min) using a dielectric barrier discharge configuration both with He-only gas as well as with He/H2 gas mixtures, yielding small NPs (< 30 nm diameter). To prove the practical utility of exsolved NPs, we have carried out various experiments aimed at assessing their catalytic performance for methanation from synthesis gas, CO and CH4 oxidation. We successfully demonstrated low-temperature and atmospheric pressure plasma exsolution and suggest that this approach could contribute to the practical deployment of exsolution-based stable catalyst systems.

KW - nanoparticles

KW - perovskite oxides

KW - catalyst-support systems

KW - exsolution

KW - dielectric barrier discharge

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VL - 11

JO - Advanced Science

JF - Advanced Science

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M1 - 2402235

ER -

Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure

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Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure

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Data for: "Dielectric barrier plasma discharge exsolution of nanoparticles at room temperature and atmospheric pressure"

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