A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles

Autores
Puszkiel, Julián Atilio; Castro Riglos, Maria Victoria; Ramallo Lopez, Jose Martin; Mizrahi, Martin Daniel; Karimi, F.; Santoru, Antonio; Hoell, Armin; Gennari, Fabiana Cristina; Arneodo Larochette, Pierre Paul; Pistidda, Claudio; Klassen, Thomas; Bellosta Von Colbe, J.M.; Dornheim, M.
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Aiming to improve the hydrogen storage properties of 2LiH + MgB2 (Li-RHC), the effect of TiO2 addition to Li-RHC is investigated. The presence of TiO2 leads to the in situ formation of core-shell LixTiO2 nanoparticles during milling and upon heating. These nanoparticles markedly enhance the hydrogen storage properties of Li-RHC. Throughout hydrogenation-dehydrogenation cycling at 400 °C a 1 mol% TiO2 doped Li-RHC material shows sustainable hydrogen capacity of ∼10 wt% and short hydrogenation and dehydrogenation times of just 25 and 50 minutes, respectively. The in situ formed core-shell LixTiO2 nanoparticles confer proper microstructural refinement to the Li-RHC, thus preventing the material's agglomeration upon cycling. An analysis of the kinetic mechanisms shows that the presence of the core-shell LixTiO2 nanoparticles accelerates the one-dimensional interface-controlled mechanism during hydrogenation owing to the high Li+ mobility through the LixTiO2 lattice. Upon dehydrogenation, the in situ formed core-shell LixTiO2 nanoparticles do not modify the dehydrogenation thermodynamic properties of the Li-RHC itself. A new approach by the combination of two kinetic models evidences that the activation energy of both MgH2 decomposition and MgB2 formation is reduced. These improvements are due to a novel catalytic mechanism via Li+ source/sink reversible reactions.
Fil: Puszkiel, Julián Atilio. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Helmholtz–Zentrum Geesthacht; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Castro Riglos, Maria Victoria. Comision Nacional de Energía Atómica. Gerencia de Área Investigaciones y Aplicaciones no Nucleares. Gerencia de Física (Centro Atómico Bariloche). División Física de Metales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Ramallo Lopez, Jose Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Karimi, F.. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Santoru, Antonio. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Hoell, Armin. Helmholtz-zentrum Berlin; Alemania
Fil: Gennari, Fabiana Cristina. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Arneodo Larochette, Pierre Paul. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Pistidda, Claudio. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Klassen, Thomas. Helmut Schmidt University; Alemania
Fil: Bellosta Von Colbe, J.M.. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Dornheim, M.. Helmholtz–Zentrum Geesthacht; Alemania
Materia
HYDROGEN STOREGE
CORESHELL NANOPARTICLES
TiO2
XANES
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/125958
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/125958
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticlesPuszkiel, Julián AtilioCastro Riglos, Maria VictoriaRamallo Lopez, Jose MartinMizrahi, Martin DanielKarimi, F.Santoru, AntonioHoell, ArminGennari, Fabiana CristinaArneodo Larochette, Pierre PaulPistidda, ClaudioKlassen, ThomasBellosta Von Colbe, J.M.Dornheim, M.HYDROGEN STOREGECORESHELL NANOPARTICLESTiO2XANEShttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2Aiming to improve the hydrogen storage properties of 2LiH + MgB2 (Li-RHC), the effect of TiO2 addition to Li-RHC is investigated. The presence of TiO2 leads to the in situ formation of core-shell LixTiO2 nanoparticles during milling and upon heating. These nanoparticles markedly enhance the hydrogen storage properties of Li-RHC. Throughout hydrogenation-dehydrogenation cycling at 400 °C a 1 mol% TiO2 doped Li-RHC material shows sustainable hydrogen capacity of ∼10 wt% and short hydrogenation and dehydrogenation times of just 25 and 50 minutes, respectively. The in situ formed core-shell LixTiO2 nanoparticles confer proper microstructural refinement to the Li-RHC, thus preventing the material's agglomeration upon cycling. An analysis of the kinetic mechanisms shows that the presence of the core-shell LixTiO2 nanoparticles accelerates the one-dimensional interface-controlled mechanism during hydrogenation owing to the high Li+ mobility through the LixTiO2 lattice. Upon dehydrogenation, the in situ formed core-shell LixTiO2 nanoparticles do not modify the dehydrogenation thermodynamic properties of the Li-RHC itself. A new approach by the combination of two kinetic models evidences that the activation energy of both MgH2 decomposition and MgB2 formation is reduced. These improvements are due to a novel catalytic mechanism via Li+ source/sink reversible reactions.Fil: Puszkiel, Julián Atilio. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Helmholtz–Zentrum Geesthacht; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Castro Riglos, Maria Victoria. Comision Nacional de Energía Atómica. Gerencia de Área Investigaciones y Aplicaciones no Nucleares. Gerencia de Física (Centro Atómico Bariloche). División Física de Metales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Ramallo Lopez, Jose Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Karimi, F.. Helmholtz–Zentrum Geesthacht; AlemaniaFil: Santoru, Antonio. Helmholtz–Zentrum Geesthacht; AlemaniaFil: Hoell, Armin. Helmholtz-zentrum Berlin; AlemaniaFil: Gennari, Fabiana Cristina. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Arneodo Larochette, Pierre Paul. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Pistidda, Claudio. Helmholtz–Zentrum Geesthacht; AlemaniaFil: Klassen, Thomas. Helmut Schmidt University; AlemaniaFil: Bellosta Von Colbe, J.M.. Helmholtz–Zentrum Geesthacht; AlemaniaFil: Dornheim, M.. Helmholtz–Zentrum Geesthacht; AlemaniaRoyal Society of Chemistry2017-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/125958Puszkiel, Julián Atilio; Castro Riglos, Maria Victoria; Ramallo Lopez, Jose Martin; Mizrahi, Martin Daniel; Karimi, F.; et al.; A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles; Royal Society of Chemistry; Journal of Materials Chemistry A; 5; 25; 5-2017; 12922-129332050-74882050-7496CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2017/ta/c7ta03117c#!divAbstractinfo:eu-repo/semantics/altIdentifier/doi/10.1039/C7TA03117Cinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:58:40Zoai:ri.conicet.gov.ar:11336/125958instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-15 14:58:40.708CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
title A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
spellingShingle A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
Puszkiel, Julián Atilio
HYDROGEN STOREGE
CORESHELL NANOPARTICLES
TiO2
XANES
title_short A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
title_full A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
title_fullStr A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
title_full_unstemmed A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
title_sort A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles
dc.creator.none.fl_str_mv Puszkiel, Julián Atilio
Castro Riglos, Maria Victoria
Ramallo Lopez, Jose Martin
Mizrahi, Martin Daniel
Karimi, F.
Santoru, Antonio
Hoell, Armin
Gennari, Fabiana Cristina
Arneodo Larochette, Pierre Paul
Pistidda, Claudio
Klassen, Thomas
Bellosta Von Colbe, J.M.
Dornheim, M.
author Puszkiel, Julián Atilio
author_facet Puszkiel, Julián Atilio
Castro Riglos, Maria Victoria
Ramallo Lopez, Jose Martin
Mizrahi, Martin Daniel
Karimi, F.
Santoru, Antonio
Hoell, Armin
Gennari, Fabiana Cristina
Arneodo Larochette, Pierre Paul
Pistidda, Claudio
Klassen, Thomas
Bellosta Von Colbe, J.M.
Dornheim, M.
author_role author
author2 Castro Riglos, Maria Victoria
Ramallo Lopez, Jose Martin
Mizrahi, Martin Daniel
Karimi, F.
Santoru, Antonio
Hoell, Armin
Gennari, Fabiana Cristina
Arneodo Larochette, Pierre Paul
Pistidda, Claudio
Klassen, Thomas
Bellosta Von Colbe, J.M.
Dornheim, M.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv HYDROGEN STOREGE
CORESHELL NANOPARTICLES
TiO2
XANES
topic HYDROGEN STOREGE
CORESHELL NANOPARTICLES
TiO2
XANES
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Aiming to improve the hydrogen storage properties of 2LiH + MgB2 (Li-RHC), the effect of TiO2 addition to Li-RHC is investigated. The presence of TiO2 leads to the in situ formation of core-shell LixTiO2 nanoparticles during milling and upon heating. These nanoparticles markedly enhance the hydrogen storage properties of Li-RHC. Throughout hydrogenation-dehydrogenation cycling at 400 °C a 1 mol% TiO2 doped Li-RHC material shows sustainable hydrogen capacity of ∼10 wt% and short hydrogenation and dehydrogenation times of just 25 and 50 minutes, respectively. The in situ formed core-shell LixTiO2 nanoparticles confer proper microstructural refinement to the Li-RHC, thus preventing the material's agglomeration upon cycling. An analysis of the kinetic mechanisms shows that the presence of the core-shell LixTiO2 nanoparticles accelerates the one-dimensional interface-controlled mechanism during hydrogenation owing to the high Li+ mobility through the LixTiO2 lattice. Upon dehydrogenation, the in situ formed core-shell LixTiO2 nanoparticles do not modify the dehydrogenation thermodynamic properties of the Li-RHC itself. A new approach by the combination of two kinetic models evidences that the activation energy of both MgH2 decomposition and MgB2 formation is reduced. These improvements are due to a novel catalytic mechanism via Li+ source/sink reversible reactions.
Fil: Puszkiel, Julián Atilio. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Helmholtz–Zentrum Geesthacht; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Castro Riglos, Maria Victoria. Comision Nacional de Energía Atómica. Gerencia de Área Investigaciones y Aplicaciones no Nucleares. Gerencia de Física (Centro Atómico Bariloche). División Física de Metales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Ramallo Lopez, Jose Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Karimi, F.. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Santoru, Antonio. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Hoell, Armin. Helmholtz-zentrum Berlin; Alemania
Fil: Gennari, Fabiana Cristina. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Arneodo Larochette, Pierre Paul. Comision Nacional de Energia Atomica. Gerencia D/area de Energia Nuclear. Gerencia Materiales.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Pistidda, Claudio. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Klassen, Thomas. Helmut Schmidt University; Alemania
Fil: Bellosta Von Colbe, J.M.. Helmholtz–Zentrum Geesthacht; Alemania
Fil: Dornheim, M.. Helmholtz–Zentrum Geesthacht; Alemania
description Aiming to improve the hydrogen storage properties of 2LiH + MgB2 (Li-RHC), the effect of TiO2 addition to Li-RHC is investigated. The presence of TiO2 leads to the in situ formation of core-shell LixTiO2 nanoparticles during milling and upon heating. These nanoparticles markedly enhance the hydrogen storage properties of Li-RHC. Throughout hydrogenation-dehydrogenation cycling at 400 °C a 1 mol% TiO2 doped Li-RHC material shows sustainable hydrogen capacity of ∼10 wt% and short hydrogenation and dehydrogenation times of just 25 and 50 minutes, respectively. The in situ formed core-shell LixTiO2 nanoparticles confer proper microstructural refinement to the Li-RHC, thus preventing the material's agglomeration upon cycling. An analysis of the kinetic mechanisms shows that the presence of the core-shell LixTiO2 nanoparticles accelerates the one-dimensional interface-controlled mechanism during hydrogenation owing to the high Li+ mobility through the LixTiO2 lattice. Upon dehydrogenation, the in situ formed core-shell LixTiO2 nanoparticles do not modify the dehydrogenation thermodynamic properties of the Li-RHC itself. A new approach by the combination of two kinetic models evidences that the activation energy of both MgH2 decomposition and MgB2 formation is reduced. These improvements are due to a novel catalytic mechanism via Li+ source/sink reversible reactions.
publishDate 2017
dc.date.none.fl_str_mv 2017-05
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/125958
Puszkiel, Julián Atilio; Castro Riglos, Maria Victoria; Ramallo Lopez, Jose Martin; Mizrahi, Martin Daniel; Karimi, F.; et al.; A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles; Royal Society of Chemistry; Journal of Materials Chemistry A; 5; 25; 5-2017; 12922-12933
2050-7488
2050-7496
CONICET Digital
CONICET
url http://hdl.handle.net/11336/125958
identifier_str_mv Puszkiel, Julián Atilio; Castro Riglos, Maria Victoria; Ramallo Lopez, Jose Martin; Mizrahi, Martin Daniel; Karimi, F.; et al.; A novel catalytic route for hydrogenation-dehydrogenation of 2LiH + MgB2: Via in situ formed core-shell LixTiO2 nanoparticles; Royal Society of Chemistry; Journal of Materials Chemistry A; 5; 25; 5-2017; 12922-12933
2050-7488
2050-7496
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2017/ta/c7ta03117c#!divAbstract
info:eu-repo/semantics/altIdentifier/doi/10.1039/C7TA03117C
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.22299

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