Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions

Current studies on ammonia synthesis by means of atmospheric pressure plasmas respond to the urgent need of developing less environmentally aggressive processes than the conventional Haber-Bosch catalytic reaction. Herein, we systematically study the plasma synthesis of ammonia and the much less inv...

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Autores: Navascués, Paula, Obrero Pérez, José M., Cotrino Bautista, José, González-Elipe, Agustín R., Gómez Ramírez, Ana María
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2020
País:España
Institución:Universidad de Sevilla (US)
Repositorio:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/143260
Acceso en línea:https://hdl.handle.net/11441/143260
https://doi.org/10.1021/acssuschemeng.0c04461
Access Level:acceso abierto
Palabra clave:Ammonia synthesis
Atmospheric pressure plasma
Energy efficiency
Ferroelectric materials
Hydrogen production
Inefficient plasma processes
Packed-bed plasma reactors
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spelling Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia ReactionsNavascués, PaulaObrero Pérez, José M.Cotrino Bautista, JoséGonzález-Elipe, Agustín R.Gómez Ramírez, Ana MaríaAmmonia synthesisAtmospheric pressure plasmaEnergy efficiencyFerroelectric materialsHydrogen productionInefficient plasma processesPacked-bed plasma reactorsCurrent studies on ammonia synthesis by means of atmospheric pressure plasmas respond to the urgent need of developing less environmentally aggressive processes than the conventional Haber-Bosch catalytic reaction. Herein, we systematically study the plasma synthesis of ammonia and the much less investigated reverse reaction (decomposition of ammonia into nitrogen and hydrogen). Besides analyzing the efficiency of both processes in a packed-bed plasma reactor, we apply an isotope-exchange approach (using D2 instead of H2) to study the reaction mechanisms. Isotope labeling has been rarely applied to investigate atmospheric plasma reactions, and we demonstrate that this methodology may provide unique information about intermediate reactions that, consuming energy and diminishing the process efficiency, do not effectively contribute to the overall synthesis/decomposition of ammonia. In addition, the same methodology has demonstrated the active participation of the interelectrode material surface in the plasma-activated synthesis/decomposition of ammonia. These results about the involvement of surface reactions in packed-bed plasma processes, complemented with data obtained by optical emission spectroscopy analysis of the plasma phase, have evidenced the occurrence of inefficient intermediate reaction mechanisms that limit the efficiency and shown that the rate-limiting step for the ammonia synthesis and decomposition reactions are the formation of NH∗ species in the plasma phase and the electron impact dissociation of the molecule, respectively.Ministerio de Economía y Competitividad MAT2016-79866-R, 201860E05Junta de Andalucía P12-2265, US-1263142American Chemical SocietyFísica Atómica, Molecular y NuclearMinisterio de Economía y Competitividad (MINECO). EspañaJunta de Andalucía2020info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfapplication/pdfhttps://hdl.handle.net/11441/143260https://doi.org/10.1021/acssuschemeng.0c04461reponame:idUS. Depósito de Investigación de la Universidad de Sevillainstname:Universidad de Sevilla (US)InglésACS Sustainable Chemistry and Engineering, 8 (39), 14855-14866.MAT2016-79866-R201860E05P12-2265US-1263142https://dx.doi.org/10.1021/acssuschemeng.0c04461info:eu-repo/semantics/openAccessoai:idus.us.es:11441/1432602026-06-17T12:51:07Z
dc.title.none.fl_str_mv Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
title Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
spellingShingle Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
Navascués, Paula
Ammonia synthesis
Atmospheric pressure plasma
Energy efficiency
Ferroelectric materials
Hydrogen production
Inefficient plasma processes
Packed-bed plasma reactors
title_short Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
title_full Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
title_fullStr Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
title_full_unstemmed Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
title_sort Unraveling Discharge and Surface Mechanisms in Plasma-Assisted Ammonia Reactions
dc.creator.none.fl_str_mv Navascués, Paula
Obrero Pérez, José M.
Cotrino Bautista, José
González-Elipe, Agustín R.
Gómez Ramírez, Ana María
author Navascués, Paula
author_facet Navascués, Paula
Obrero Pérez, José M.
Cotrino Bautista, José
González-Elipe, Agustín R.
Gómez Ramírez, Ana María
author_role author
author2 Obrero Pérez, José M.
Cotrino Bautista, José
González-Elipe, Agustín R.
Gómez Ramírez, Ana María
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Física Atómica, Molecular y Nuclear
Ministerio de Economía y Competitividad (MINECO). España
Junta de Andalucía
dc.subject.none.fl_str_mv Ammonia synthesis
Atmospheric pressure plasma
Energy efficiency
Ferroelectric materials
Hydrogen production
Inefficient plasma processes
Packed-bed plasma reactors
topic Ammonia synthesis
Atmospheric pressure plasma
Energy efficiency
Ferroelectric materials
Hydrogen production
Inefficient plasma processes
Packed-bed plasma reactors
description Current studies on ammonia synthesis by means of atmospheric pressure plasmas respond to the urgent need of developing less environmentally aggressive processes than the conventional Haber-Bosch catalytic reaction. Herein, we systematically study the plasma synthesis of ammonia and the much less investigated reverse reaction (decomposition of ammonia into nitrogen and hydrogen). Besides analyzing the efficiency of both processes in a packed-bed plasma reactor, we apply an isotope-exchange approach (using D2 instead of H2) to study the reaction mechanisms. Isotope labeling has been rarely applied to investigate atmospheric plasma reactions, and we demonstrate that this methodology may provide unique information about intermediate reactions that, consuming energy and diminishing the process efficiency, do not effectively contribute to the overall synthesis/decomposition of ammonia. In addition, the same methodology has demonstrated the active participation of the interelectrode material surface in the plasma-activated synthesis/decomposition of ammonia. These results about the involvement of surface reactions in packed-bed plasma processes, complemented with data obtained by optical emission spectroscopy analysis of the plasma phase, have evidenced the occurrence of inefficient intermediate reaction mechanisms that limit the efficiency and shown that the rate-limiting step for the ammonia synthesis and decomposition reactions are the formation of NH∗ species in the plasma phase and the electron impact dissociation of the molecule, respectively.
publishDate 2020
dc.date.none.fl_str_mv 2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/11441/143260
https://doi.org/10.1021/acssuschemeng.0c04461
url https://hdl.handle.net/11441/143260
https://doi.org/10.1021/acssuschemeng.0c04461
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv ACS Sustainable Chemistry and Engineering, 8 (39), 14855-14866.
MAT2016-79866-R
201860E05
P12-2265
US-1263142
https://dx.doi.org/10.1021/acssuschemeng.0c04461
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:idUS. Depósito de Investigación de la Universidad de Sevilla
instname:Universidad de Sevilla (US)
instname_str Universidad de Sevilla (US)
reponame_str idUS. Depósito de Investigación de la Universidad de Sevilla
collection idUS. Depósito de Investigación de la Universidad de Sevilla
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300719

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