N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation

Detalhes bibliográficos
Autor(a) principal: Chatain, Audrey
Data de Publicação: 2020
Outros Autores: Jiménez-Redondo, Miguel, Vettier, Ludovic, Guaitella, Olivier, Carrasco, Nathalie, Alves, Luis Lemos, Marques, L., Cernogora, Guy
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/1822/68888
Resumo: The mixing of N2 with H2 leads to very different plasmas from pure N2 and H2 plasma discharges. Numerous issues are therefore raised involving the processes leading to ammonia (NH3) formation. The aim of this work is to better characterize capacitively-coupled radiofrequency plasma discharges in N2 with few percents of H2 (up to 5%), at low pressure (0.3-1 mbar) and low coupled power (3-13 W). Both experimental measurements and numerical simulations are performed. For clarity, we separated the results in two complementary parts. The actual one (first part), presents the details on the experimental measurements, while the second focuses on the simulation, a hybrid model combining a 2D fluid module and a 0D kinetic module. Electron density is measured by a resonant cavity method. It varies from 0.4 to 5 109 cm-3, corresponding to ionization degrees from 2 10-8 to 4 10-7. Ammonia density is quantified by combining IR absorption and mass spectrometry. It increases linearly with the amount of H2 (up to 3 1013 cm-3 at 5% H2). On the contrary, it is constant with pressure, which suggests the dominance of surface processes on the formation of ammonia. Positive ions are measured by mass spectrometry. Nitrogen-bearing ions are hydrogenated by the injection of H2, N2H+ being the major ion as soon as the amount of H2 is >1%. The increase of pressure leads to an increase of secondary ions formed by ion/radical-neutral collisions (ex: N2H+, NH4 +, H3 +), while an increase of the coupled power favours ions formed by direct ionization (ex: N2 +, NH3 +, H2 +).
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spelling N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formationcold plasmaCCP dischargeN-2-H(2)mixtureNH3IR absorptionneutral and ion mass spectrometryplasma surface interactionsCiências Naturais::Ciências FísicasScience & TechnologyThe mixing of N2 with H2 leads to very different plasmas from pure N2 and H2 plasma discharges. Numerous issues are therefore raised involving the processes leading to ammonia (NH3) formation. The aim of this work is to better characterize capacitively-coupled radiofrequency plasma discharges in N2 with few percents of H2 (up to 5%), at low pressure (0.3-1 mbar) and low coupled power (3-13 W). Both experimental measurements and numerical simulations are performed. For clarity, we separated the results in two complementary parts. The actual one (first part), presents the details on the experimental measurements, while the second focuses on the simulation, a hybrid model combining a 2D fluid module and a 0D kinetic module. Electron density is measured by a resonant cavity method. It varies from 0.4 to 5 109 cm-3, corresponding to ionization degrees from 2 10-8 to 4 10-7. Ammonia density is quantified by combining IR absorption and mass spectrometry. It increases linearly with the amount of H2 (up to 3 1013 cm-3 at 5% H2). On the contrary, it is constant with pressure, which suggests the dominance of surface processes on the formation of ammonia. Positive ions are measured by mass spectrometry. Nitrogen-bearing ions are hydrogenated by the injection of H2, N2H+ being the major ion as soon as the amount of H2 is >1%. The increase of pressure leads to an increase of secondary ions formed by ion/radical-neutral collisions (ex: N2H+, NH4 +, H3 +), while an increase of the coupled power favours ions formed by direct ionization (ex: N2 +, NH3 +, H2 +).N. Carrasco acknowledges the financial support of the European Research Council (ERC Starting Grant PRIMCHEM, Grant agreement no. 636829). A. Chatain acknowledges ENS Paris-Saclay Doctoral Program. A. Chatain is grateful to Gilles Cartry and Thomas Gautier for fruitful discussions on the MS calibration. L.L. Alves acknowledges the financial support of the Portuguese Foundation for Science and Technology (FCT) through the project UID/FIS/50010/2019. L. Marques and M. J. Redondo acknowledge the financial support of the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Funding UIDB/04650/2019.IOP PublishingUniversidade do MinhoChatain, AudreyJiménez-Redondo, MiguelVettier, LudovicGuaitella, OlivierCarrasco, NathalieAlves, Luis LemosMarques, L.Cernogora, Guy20202020-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/1822/68888eng0963-025210.1088/1361-6595/ab9b1ahttps://iopscience.iop.org/article/10.1088/1361-6595/ab9b1ainfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2023-07-21T12:37:45Zoai:repositorium.sdum.uminho.pt:1822/68888Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T19:34:08.141671Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse
dc.title.none.fl_str_mv N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
title N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
spellingShingle N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
Chatain, Audrey
cold plasma
CCP discharge
N-2-H(2)mixture
NH3
IR absorption
neutral and ion mass spectrometry
plasma surface interactions
Ciências Naturais::Ciências Físicas
Science & Technology
title_short N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
title_full N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
title_fullStr N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
title_full_unstemmed N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
title_sort N2-H2 capacitively coupled radio-frequency discharges at low pressure. Part I. Experimental results: Effect of the H2 amount on electrons, positive ions and ammonia formation
author Chatain, Audrey
author_facet Chatain, Audrey
Jiménez-Redondo, Miguel
Vettier, Ludovic
Guaitella, Olivier
Carrasco, Nathalie
Alves, Luis Lemos
Marques, L.
Cernogora, Guy
author_role author
author2 Jiménez-Redondo, Miguel
Vettier, Ludovic
Guaitella, Olivier
Carrasco, Nathalie
Alves, Luis Lemos
Marques, L.
Cernogora, Guy
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Universidade do Minho
dc.contributor.author.fl_str_mv Chatain, Audrey
Jiménez-Redondo, Miguel
Vettier, Ludovic
Guaitella, Olivier
Carrasco, Nathalie
Alves, Luis Lemos
Marques, L.
Cernogora, Guy
dc.subject.por.fl_str_mv cold plasma
CCP discharge
N-2-H(2)mixture
NH3
IR absorption
neutral and ion mass spectrometry
plasma surface interactions
Ciências Naturais::Ciências Físicas
Science & Technology
topic cold plasma
CCP discharge
N-2-H(2)mixture
NH3
IR absorption
neutral and ion mass spectrometry
plasma surface interactions
Ciências Naturais::Ciências Físicas
Science & Technology
description The mixing of N2 with H2 leads to very different plasmas from pure N2 and H2 plasma discharges. Numerous issues are therefore raised involving the processes leading to ammonia (NH3) formation. The aim of this work is to better characterize capacitively-coupled radiofrequency plasma discharges in N2 with few percents of H2 (up to 5%), at low pressure (0.3-1 mbar) and low coupled power (3-13 W). Both experimental measurements and numerical simulations are performed. For clarity, we separated the results in two complementary parts. The actual one (first part), presents the details on the experimental measurements, while the second focuses on the simulation, a hybrid model combining a 2D fluid module and a 0D kinetic module. Electron density is measured by a resonant cavity method. It varies from 0.4 to 5 109 cm-3, corresponding to ionization degrees from 2 10-8 to 4 10-7. Ammonia density is quantified by combining IR absorption and mass spectrometry. It increases linearly with the amount of H2 (up to 3 1013 cm-3 at 5% H2). On the contrary, it is constant with pressure, which suggests the dominance of surface processes on the formation of ammonia. Positive ions are measured by mass spectrometry. Nitrogen-bearing ions are hydrogenated by the injection of H2, N2H+ being the major ion as soon as the amount of H2 is >1%. The increase of pressure leads to an increase of secondary ions formed by ion/radical-neutral collisions (ex: N2H+, NH4 +, H3 +), while an increase of the coupled power favours ions formed by direct ionization (ex: N2 +, NH3 +, H2 +).
publishDate 2020
dc.date.none.fl_str_mv 2020
2020-01-01T00:00:00Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://hdl.handle.net/1822/68888
url http://hdl.handle.net/1822/68888
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 0963-0252
10.1088/1361-6595/ab9b1a
https://iopscience.iop.org/article/10.1088/1361-6595/ab9b1a
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv IOP Publishing
publisher.none.fl_str_mv IOP Publishing
dc.source.none.fl_str_mv reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
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instacron_str RCAAP
institution RCAAP
reponame_str Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
collection Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
repository.name.fl_str_mv Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
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