Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature

Hessan Khalid; Atta ul Haq; Bruno Alessi; Ji Wu; Cristian D. Savaniu; Kalliopi Kousi; Ian S. Metcalfe; Stephen C. Parker; John Thomas Sirr Irvine; Paul Maguire; Evangelos I. Papaioannou; Davide Mariotti

doi:10.1002/aenm.202201131

Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature

Hessan Khalid, Atta ul Haq, Bruno Alessi, Ji Wu, Cristian D. Savaniu, Kalliopi Kousi, Ian S. Metcalfe, Stephen C. Parker, John Thomas Sirr Irvine, Paul Maguire, Evangelos I. Papaioannou, Davide Mariotti

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Abstract

High-performance nanoparticle platforms can drive catalysis progress to new horizons, delivering environmental and energy targets. Nanoparticle exsolution offers unprecedented opportunities that are limited by current demanding process conditions. Unraveling new exsolution pathways, particularly at low-temperatures, represents an important milestone that will enable improved sustainable synthetic route, more control of catalysis microstructure as well as new application opportunities. Herein it is demonstrated that plasma direct exsolution at room temperature represents just such a step change in the synthesis. Moreover, the factors that most affect the exsolution process are identified. It is shown that the surface defects produced initiate exsolution under a brief ion bombardment of an argon low-pressure and low-temperature plasma. This results in controlled nanoparticles with diameters ≈19–22 nm with very high number densities thus creating a highly active catalytic material for CO oxidation which rivals traditionally created exsolved samples.

Original language	English
Article number	2201131
Journal	Advanced Energy Materials
Volume	12
Issue number	45
Early online date	3 Oct 2022
DOIs	https://doi.org/10.1002/aenm.202201131
Publication status	Published online - 3 Oct 2022

Bibliographical note

Funding Information:
The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

Publisher Copyright:
© 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.

Funding Information:
The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

Funding Information:
The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath.

Publisher Copyright:
© 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.

Funding

Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: © 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: © 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.

Keywords

exsolution
perovskite oxide

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/aenm.202201131

aenm.202201131Final published version, 2.45 MBLicence: CC BY

Cite this

Khalid, H., Haq, A. U., Alessi, B., Wu, J., Savaniu, C. D., Kousi, K., Metcalfe, I. S., Parker, S. C., Irvine, J. T. S., Maguire, P., Papaioannou, E. I., & Mariotti, D. (2022). Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature. Advanced Energy Materials, 12(45), Article 2201131. Advance online publication. https://doi.org/10.1002/aenm.202201131

@article{f32c9a494eeb4b8089f22324fbc8c68d,

title = "Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature",

abstract = "High-performance nanoparticle platforms can drive catalysis progress to new horizons, delivering environmental and energy targets. Nanoparticle exsolution offers unprecedented opportunities that are limited by current demanding process conditions. Unraveling new exsolution pathways, particularly at low-temperatures, represents an important milestone that will enable improved sustainable synthetic route, more control of catalysis microstructure as well as new application opportunities. Herein it is demonstrated that plasma direct exsolution at room temperature represents just such a step change in the synthesis. Moreover, the factors that most affect the exsolution process are identified. It is shown that the surface defects produced initiate exsolution under a brief ion bombardment of an argon low-pressure and low-temperature plasma. This results in controlled nanoparticles with diameters ≈19–22 nm with very high number densities thus creating a highly active catalytic material for CO oxidation which rivals traditionally created exsolved samples.",

keywords = "exsolution, perovskite oxide",

author = "Hessan Khalid and Haq, \{Atta ul\} and Bruno Alessi and Ji Wu and Savaniu, \{Cristian D.\} and Kalliopi Kousi and Metcalfe, \{Ian S.\} and Parker, \{Stephen C.\} and Irvine, \{John Thomas Sirr\} and Paul Maguire and Papaioannou, \{Evangelos I.\} and Davide Mariotti",

note = "Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.",

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AU - Haq, Atta ul

AU - Alessi, Bruno

AU - Wu, Ji

AU - Savaniu, Cristian D.

AU - Kousi, Kalliopi

AU - Metcalfe, Ian S.

AU - Parker, Stephen C.

AU - Irvine, John Thomas Sirr

AU - Maguire, Paul

AU - Papaioannou, Evangelos I.

AU - Mariotti, Davide

N1 - Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: © 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Funding Information: The research was supported by EPSRC (Award Nos. EP/R023522/1, EP/R023603/1, EP/R023921/1, EP/R023638/1, EP/R008841/1, and EP/V055232/1) and financial support from the UK Catalysis Hub funded by EPSRC Grant reference EP/R027129/1. J.W. and S.C.P. gratefully acknowledge support from the EPSRC (EP/P007821/1) and also thank the U.K. ARCHER HPC facility and the THOMAS HPC (the UK Materials and Molecular Modelling Hub, partially funded by EPSRC EP/P020194) for providing computation resources, via the membership of the UK's HEC Materials Chemistry Consortium (funded by the EPSRC Grant Nos. EP/L000202, EP/709 P007821/1, EP/R029431, and EP/T022213). This research has also made use of the Balena High Performance Computing (HPC) Service at the University of Bath. Publisher Copyright: © 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.

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Y1 - 2022/10/3

N2 - High-performance nanoparticle platforms can drive catalysis progress to new horizons, delivering environmental and energy targets. Nanoparticle exsolution offers unprecedented opportunities that are limited by current demanding process conditions. Unraveling new exsolution pathways, particularly at low-temperatures, represents an important milestone that will enable improved sustainable synthetic route, more control of catalysis microstructure as well as new application opportunities. Herein it is demonstrated that plasma direct exsolution at room temperature represents just such a step change in the synthesis. Moreover, the factors that most affect the exsolution process are identified. It is shown that the surface defects produced initiate exsolution under a brief ion bombardment of an argon low-pressure and low-temperature plasma. This results in controlled nanoparticles with diameters ≈19–22 nm with very high number densities thus creating a highly active catalytic material for CO oxidation which rivals traditionally created exsolved samples.

AB - High-performance nanoparticle platforms can drive catalysis progress to new horizons, delivering environmental and energy targets. Nanoparticle exsolution offers unprecedented opportunities that are limited by current demanding process conditions. Unraveling new exsolution pathways, particularly at low-temperatures, represents an important milestone that will enable improved sustainable synthetic route, more control of catalysis microstructure as well as new application opportunities. Herein it is demonstrated that plasma direct exsolution at room temperature represents just such a step change in the synthesis. Moreover, the factors that most affect the exsolution process are identified. It is shown that the surface defects produced initiate exsolution under a brief ion bombardment of an argon low-pressure and low-temperature plasma. This results in controlled nanoparticles with diameters ≈19–22 nm with very high number densities thus creating a highly active catalytic material for CO oxidation which rivals traditionally created exsolved samples.

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IS - 45

M1 - 2201131

ER -

Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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Plasma driven exsolution from perovskite oxide for catalytic application

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Rapid Plasma Exsolution from an A-site Deficient Perovskite Oxide at Room Temperature

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Student theses

Plasma driven exsolution from perovskite oxide for catalytic application

Cite this