Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S

Autores
Braun, Fernando; Tarditi, Ana Maria; Miller, James B.; Cornaglia, Laura Maria
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Pd, Pd90Ag10, Pd91Au9, Pd78Ag9Au13 and Pd75Ag16Au9 alloy membranes were prepared on vacuum-assisted ZrO2-modified porous stainless steel supports by sequential electroless deposition. The membranes were evaluated for permeability in pure H2 and in an H2S/H2 mixture. The membranes displayed a range of permeabilities in pure H2: Pd90Ag10>Pd78Ag9Au13>Pd~Pd75Ag16Au9>Pd91Au9. On exposure to 100 ppm H2S/H2 at 673 K for 24 h, all membranes lost a significant fraction of their H2 permeabilities: Pd (lost the largest fraction, 85%)>Pd90Ag10>Pd75Ag16Au9>Pd78Ag9Au13>Pd91Au9 (60%). When H2S was removed, the membranes recovered the lost permeability to different extents. The Pd91Au9 and Pd78Ag9Au13 membranes displayed the highest fractional recovery of initial H2 permeability (~80%). But, with its higher initial pure H2 permeability, Pd78Ag9Au13 had the highest absolute H2 permeability after recovery. The microstructure, morphology and bulk composition of H2S-exposed samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). XRD revealed the presence of a bulk Pd4S phase on both Pd and Pd90Ag10, the membranes that recovered the least H2 relative flux after their exposure to H2S. In contrast, bulk sulfides did not form on Pd91Au9 or on PdAgAu ternary alloys. In agreement with the XRD results, EDS did not detect sulfur in the bulk of Pd91Au9 or in either of the ternary alloy samples. Our results show that the addition of Au to the high-permeability PdAg binary membrane results in a PdAgAu ternary membrane that minimizes the permanent H2 flux loss associated with H2S exposure by preventing the formation of thick stable sulfides.
Fil: Braun, Fernando. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Tarditi, Ana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Miller, James B.. University of Carnegie Mellon. Department of Chemical Engineering; Estados Unidos. United States Department of Energy; Estados Unidos
Fil: Cornaglia, Laura Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Materia
Pd Ternary Alloy Membrane
H2 Purification
Sulfur Tolerance
Pdagau Alloy
Hydrogen Separation Membrane
Ternary Alloy
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:11336/31709
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/31709
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2SBraun, FernandoTarditi, Ana MariaMiller, James B.Cornaglia, Laura MariaPd Ternary Alloy MembraneH2 PurificationSulfur TolerancePdagau AlloyHydrogen Separation MembraneTernary Alloyhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Pd, Pd90Ag10, Pd91Au9, Pd78Ag9Au13 and Pd75Ag16Au9 alloy membranes were prepared on vacuum-assisted ZrO2-modified porous stainless steel supports by sequential electroless deposition. The membranes were evaluated for permeability in pure H2 and in an H2S/H2 mixture. The membranes displayed a range of permeabilities in pure H2: Pd90Ag10>Pd78Ag9Au13>Pd~Pd75Ag16Au9>Pd91Au9. On exposure to 100 ppm H2S/H2 at 673 K for 24 h, all membranes lost a significant fraction of their H2 permeabilities: Pd (lost the largest fraction, 85%)>Pd90Ag10>Pd75Ag16Au9>Pd78Ag9Au13>Pd91Au9 (60%). When H2S was removed, the membranes recovered the lost permeability to different extents. The Pd91Au9 and Pd78Ag9Au13 membranes displayed the highest fractional recovery of initial H2 permeability (~80%). But, with its higher initial pure H2 permeability, Pd78Ag9Au13 had the highest absolute H2 permeability after recovery. The microstructure, morphology and bulk composition of H2S-exposed samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). XRD revealed the presence of a bulk Pd4S phase on both Pd and Pd90Ag10, the membranes that recovered the least H2 relative flux after their exposure to H2S. In contrast, bulk sulfides did not form on Pd91Au9 or on PdAgAu ternary alloys. In agreement with the XRD results, EDS did not detect sulfur in the bulk of Pd91Au9 or in either of the ternary alloy samples. Our results show that the addition of Au to the high-permeability PdAg binary membrane results in a PdAgAu ternary membrane that minimizes the permanent H2 flux loss associated with H2S exposure by preventing the formation of thick stable sulfides.Fil: Braun, Fernando. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Tarditi, Ana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Miller, James B.. University of Carnegie Mellon. Department of Chemical Engineering; Estados Unidos. United States Department of Energy; Estados UnidosFil: Cornaglia, Laura Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaElsevier2013-09info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/31709Cornaglia, Laura Maria; Miller, James B.; Tarditi, Ana Maria; Braun, Fernando; Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S; Elsevier; Journal of Membrane Science; 450; 9-2013; 299-3070376-7388CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0376738813007448info:eu-repo/semantics/altIdentifier/doi/10.1016/j.memsci.2013.09.026info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:47:15Zoai:ri.conicet.gov.ar:11336/31709instacron: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:34982025-09-03 09:47:15.553CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
title Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
spellingShingle Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
Braun, Fernando
Pd Ternary Alloy Membrane
H2 Purification
Sulfur Tolerance
Pdagau Alloy
Hydrogen Separation Membrane
Ternary Alloy
title_short Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
title_full Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
title_fullStr Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
title_full_unstemmed Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
title_sort Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S
dc.creator.none.fl_str_mv Braun, Fernando
Tarditi, Ana Maria
Miller, James B.
Cornaglia, Laura Maria
author Braun, Fernando
author_facet Braun, Fernando
Tarditi, Ana Maria
Miller, James B.
Cornaglia, Laura Maria
author_role author
author2 Tarditi, Ana Maria
Miller, James B.
Cornaglia, Laura Maria
author2_role author
author
author
dc.subject.none.fl_str_mv Pd Ternary Alloy Membrane
H2 Purification
Sulfur Tolerance
Pdagau Alloy
Hydrogen Separation Membrane
Ternary Alloy
topic Pd Ternary Alloy Membrane
H2 Purification
Sulfur Tolerance
Pdagau Alloy
Hydrogen Separation Membrane
Ternary Alloy
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Pd, Pd90Ag10, Pd91Au9, Pd78Ag9Au13 and Pd75Ag16Au9 alloy membranes were prepared on vacuum-assisted ZrO2-modified porous stainless steel supports by sequential electroless deposition. The membranes were evaluated for permeability in pure H2 and in an H2S/H2 mixture. The membranes displayed a range of permeabilities in pure H2: Pd90Ag10>Pd78Ag9Au13>Pd~Pd75Ag16Au9>Pd91Au9. On exposure to 100 ppm H2S/H2 at 673 K for 24 h, all membranes lost a significant fraction of their H2 permeabilities: Pd (lost the largest fraction, 85%)>Pd90Ag10>Pd75Ag16Au9>Pd78Ag9Au13>Pd91Au9 (60%). When H2S was removed, the membranes recovered the lost permeability to different extents. The Pd91Au9 and Pd78Ag9Au13 membranes displayed the highest fractional recovery of initial H2 permeability (~80%). But, with its higher initial pure H2 permeability, Pd78Ag9Au13 had the highest absolute H2 permeability after recovery. The microstructure, morphology and bulk composition of H2S-exposed samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). XRD revealed the presence of a bulk Pd4S phase on both Pd and Pd90Ag10, the membranes that recovered the least H2 relative flux after their exposure to H2S. In contrast, bulk sulfides did not form on Pd91Au9 or on PdAgAu ternary alloys. In agreement with the XRD results, EDS did not detect sulfur in the bulk of Pd91Au9 or in either of the ternary alloy samples. Our results show that the addition of Au to the high-permeability PdAg binary membrane results in a PdAgAu ternary membrane that minimizes the permanent H2 flux loss associated with H2S exposure by preventing the formation of thick stable sulfides.
Fil: Braun, Fernando. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Tarditi, Ana Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Miller, James B.. University of Carnegie Mellon. Department of Chemical Engineering; Estados Unidos. United States Department of Energy; Estados Unidos
Fil: Cornaglia, Laura Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
description Pd, Pd90Ag10, Pd91Au9, Pd78Ag9Au13 and Pd75Ag16Au9 alloy membranes were prepared on vacuum-assisted ZrO2-modified porous stainless steel supports by sequential electroless deposition. The membranes were evaluated for permeability in pure H2 and in an H2S/H2 mixture. The membranes displayed a range of permeabilities in pure H2: Pd90Ag10>Pd78Ag9Au13>Pd~Pd75Ag16Au9>Pd91Au9. On exposure to 100 ppm H2S/H2 at 673 K for 24 h, all membranes lost a significant fraction of their H2 permeabilities: Pd (lost the largest fraction, 85%)>Pd90Ag10>Pd75Ag16Au9>Pd78Ag9Au13>Pd91Au9 (60%). When H2S was removed, the membranes recovered the lost permeability to different extents. The Pd91Au9 and Pd78Ag9Au13 membranes displayed the highest fractional recovery of initial H2 permeability (~80%). But, with its higher initial pure H2 permeability, Pd78Ag9Au13 had the highest absolute H2 permeability after recovery. The microstructure, morphology and bulk composition of H2S-exposed samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). XRD revealed the presence of a bulk Pd4S phase on both Pd and Pd90Ag10, the membranes that recovered the least H2 relative flux after their exposure to H2S. In contrast, bulk sulfides did not form on Pd91Au9 or on PdAgAu ternary alloys. In agreement with the XRD results, EDS did not detect sulfur in the bulk of Pd91Au9 or in either of the ternary alloy samples. Our results show that the addition of Au to the high-permeability PdAg binary membrane results in a PdAgAu ternary membrane that minimizes the permanent H2 flux loss associated with H2S exposure by preventing the formation of thick stable sulfides.
publishDate 2013
dc.date.none.fl_str_mv 2013-09
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/11336/31709
Cornaglia, Laura Maria; Miller, James B.; Tarditi, Ana Maria; Braun, Fernando; Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S; Elsevier; Journal of Membrane Science; 450; 9-2013; 299-307
0376-7388
CONICET Digital
CONICET
url http://hdl.handle.net/11336/31709
identifier_str_mv Cornaglia, Laura Maria; Miller, James B.; Tarditi, Ana Maria; Braun, Fernando; Pd-based binary and ternary alloy membranes: Morphological and perm-selective characterization in the presence of H2S; Elsevier; Journal of Membrane Science; 450; 9-2013; 299-307
0376-7388
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0376738813007448
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.memsci.2013.09.026
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
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
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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