Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation

The effect of Ga as support modifier and V as second promoter on the NiMoV/Al2O3-Ga2O3 catalyst varying the synthesis method (SG: sol–gel synthesis vs I: impregnation synthesis) was studied. The catalysts were characterized by elemental analysis, textural properties, XRD, XPS, 27Al NMR, Raman, EDX e...

Full description

Autores:
Puello-Polo, Esneyder
Reales, Yelitce P.
Marquez, Edgar
Larruded, Dunieskys G.
Costa Arzuza, Luis C.
Toloza Toloza, Carlos
Tipo de recurso:
http://purl.org/coar/resource_type/c_816b
Fecha de publicación:
2020
Institución:
Corporación Universidad de la Costa
Repositorio:
REDICUC - Repositorio CUC
Idioma:
eng
OAI Identifier:
oai:repositorio.cuc.edu.co:11323/7678
Acceso en línea:
https://hdl.handle.net/11323/7678
https://doi.org/10.1007/s10562-020-03438-y
https://repositorio.cuc.edu.co/
Palabra clave:
Gallium
Vanadium
Modified al2O3
Synthesis method
Indole hydrodenitrogenation
Rights
openAccess
License
CC0 1.0 Universal
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oai_identifier_str oai:repositorio.cuc.edu.co:11323/7678
network_acronym_str RCUC2
network_name_str REDICUC - Repositorio CUC
repository_id_str
dc.title.spa.fl_str_mv Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
title Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
spellingShingle Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
Gallium
Vanadium
Modified al2O3
Synthesis method
Indole hydrodenitrogenation
title_short Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
title_full Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
title_fullStr Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
title_full_unstemmed Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
title_sort Effect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenation
dc.creator.fl_str_mv Puello-Polo, Esneyder
Reales, Yelitce P.
Marquez, Edgar
Larruded, Dunieskys G.
Costa Arzuza, Luis C.
Toloza Toloza, Carlos
dc.contributor.author.spa.fl_str_mv Puello-Polo, Esneyder
Reales, Yelitce P.
Marquez, Edgar
Larruded, Dunieskys G.
Costa Arzuza, Luis C.
Toloza Toloza, Carlos
dc.subject.spa.fl_str_mv Gallium
Vanadium
Modified al2O3
Synthesis method
Indole hydrodenitrogenation
topic Gallium
Vanadium
Modified al2O3
Synthesis method
Indole hydrodenitrogenation
description The effect of Ga as support modifier and V as second promoter on the NiMoV/Al2O3-Ga2O3 catalyst varying the synthesis method (SG: sol–gel synthesis vs I: impregnation synthesis) was studied. The catalysts were characterized by elemental analysis, textural properties, XRD, XPS, 27Al NMR, Raman, EDX elemental mapping and HRTEM. The chemical analyses by XRF showed coincidence between experimental and theoretical values according to stoichiometric values proposed to Mo/Ni = 6 and (V + Ni)/(V + Ni + Mo) = 0.35. The sol–gel synthesis method increased the surface area by incorporation of Ga3+ ions into the Al2O3 forming Ga–O–Al bonding; whereas the impregnation synthesis leads to decrease by blocking of alumina pores, as follows NiMoV/Al2O3-Ga2O3(I) < NiMoV/Al2O3-Ga2O3(SG) < Al2O3-Ga2O3(I) < NiMo/Al2O3 < Al2O3-Ga2O3(SG) < Al2O3. The values of BJH mesopores mean size between 6.13 and 7.68 nm. XRD and XPS confirmed a bulk structure typical of (NH4)4[NiMo6O24H6]·5H2O and the presence at the surface of Mo4+, Mo6+, NixSy, NiMoS, Ni2+, Ga3+ and V5+ species, respectively. Raman showed that the sol–gel synthesis method reduces the interactions Ni-Mo sulfide-support and improvement the sulfidation degree NiMoV/Al2O3-Ga2O3(SG) as showed sulfur analysis CHONS. The largest proportion of AlO4 content using the impregnation method to add Ga was verified by 27Al solid-state MAS NMR. The EDS elemental mapping confirmed that Ni, Mo, Al, Ga, V and S are well-distributed on support. The HRTEM analysis shows that the length and stacking distribution of MoS2 crystallites varied from 5.67 to 6.01 nm and 2.46 to 2.74 when using the sol–gel and impregnation synthesis method, respectively. The catalytic results revealed that the synthesis method induced the presence of gallium on the surface influencing the dispersion V5+ species, whose effect could have some relation with strength and density of acid sites that in turn influence the dispersion of the MoS2 phase, which correlates well with the indole HDN activities. The activities as indole HDN pseudo-first-order rate constants’ values (kHDN) from 0.29 to 2.78 mol/(m2·h): NiMoV/Al2O3 < NiMoV/Al2O3-Ga2O3(I) < NiMo/Al2O3 < NiMoV/Al2O3-Ga2O3(SG). Nevertheless, the nature of the active site can be related with reaction pathways, that is, NiMoV/Al2O3-Ga2O3(SG) and NiMoV/Al2O3-Ga2O3(I) catalysts produce ECH through HIND, while NiMoV/Al2O3 and NiMo/Al2O3 produce EB by hydrogenolysis of HIND to OEA. In the regard, the Ga and V act as structural promoters in the NiMo catalysts, allowing the largest generation of NiMoS M-edge-like and BRIM sites for HDN.
publishDate 2020
dc.date.issued.none.fl_str_mv 2020
dc.date.accessioned.none.fl_str_mv 2021-01-13T21:38:10Z
dc.date.available.none.fl_str_mv 2021-01-13T21:38:10Z
dc.type.spa.fl_str_mv Pre-Publicación
dc.type.coar.spa.fl_str_mv http://purl.org/coar/resource_type/c_816b
dc.type.content.spa.fl_str_mv Text
dc.type.driver.spa.fl_str_mv info:eu-repo/semantics/preprint
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format http://purl.org/coar/resource_type/c_816b
status_str acceptedVersion
dc.identifier.issn.spa.fl_str_mv 1572-879X
1011-372X
dc.identifier.uri.spa.fl_str_mv https://hdl.handle.net/11323/7678
dc.identifier.doi.spa.fl_str_mv https://doi.org/10.1007/s10562-020-03438-y
dc.identifier.instname.spa.fl_str_mv Corporación Universidad de la Costa
dc.identifier.reponame.spa.fl_str_mv REDICUC - Repositorio CUC
dc.identifier.repourl.spa.fl_str_mv https://repositorio.cuc.edu.co/
identifier_str_mv 1572-879X
1011-372X
Corporación Universidad de la Costa
REDICUC - Repositorio CUC
url https://hdl.handle.net/11323/7678
https://doi.org/10.1007/s10562-020-03438-y
https://repositorio.cuc.edu.co/
dc.language.iso.none.fl_str_mv eng
language eng
dc.rights.spa.fl_str_mv CC0 1.0 Universal
dc.rights.uri.spa.fl_str_mv http://creativecommons.org/publicdomain/zero/1.0/
dc.rights.accessrights.spa.fl_str_mv info:eu-repo/semantics/openAccess
dc.rights.coar.spa.fl_str_mv http://purl.org/coar/access_right/c_abf2
rights_invalid_str_mv CC0 1.0 Universal
http://creativecommons.org/publicdomain/zero/1.0/
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eu_rights_str_mv openAccess
dc.format.mimetype.spa.fl_str_mv application/pdf
dc.publisher.spa.fl_str_mv Corporación Universidad de la Costa
dc.source.spa.fl_str_mv Catalysis Letters
institution Corporación Universidad de la Costa
dc.source.url.spa.fl_str_mv https://link.springer.com/article/10.1007/s10562-020-03438-y
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spelling Puello-Polo, EsneyderReales, Yelitce P.Marquez, EdgarLarruded, Dunieskys G.Costa Arzuza, Luis C.Toloza Toloza, Carlos2021-01-13T21:38:10Z2021-01-13T21:38:10Z20201572-879X1011-372Xhttps://hdl.handle.net/11323/7678https://doi.org/10.1007/s10562-020-03438-yCorporación Universidad de la CostaREDICUC - Repositorio CUChttps://repositorio.cuc.edu.co/The effect of Ga as support modifier and V as second promoter on the NiMoV/Al2O3-Ga2O3 catalyst varying the synthesis method (SG: sol–gel synthesis vs I: impregnation synthesis) was studied. The catalysts were characterized by elemental analysis, textural properties, XRD, XPS, 27Al NMR, Raman, EDX elemental mapping and HRTEM. The chemical analyses by XRF showed coincidence between experimental and theoretical values according to stoichiometric values proposed to Mo/Ni = 6 and (V + Ni)/(V + Ni + Mo) = 0.35. The sol–gel synthesis method increased the surface area by incorporation of Ga3+ ions into the Al2O3 forming Ga–O–Al bonding; whereas the impregnation synthesis leads to decrease by blocking of alumina pores, as follows NiMoV/Al2O3-Ga2O3(I) < NiMoV/Al2O3-Ga2O3(SG) < Al2O3-Ga2O3(I) < NiMo/Al2O3 < Al2O3-Ga2O3(SG) < Al2O3. The values of BJH mesopores mean size between 6.13 and 7.68 nm. XRD and XPS confirmed a bulk structure typical of (NH4)4[NiMo6O24H6]·5H2O and the presence at the surface of Mo4+, Mo6+, NixSy, NiMoS, Ni2+, Ga3+ and V5+ species, respectively. Raman showed that the sol–gel synthesis method reduces the interactions Ni-Mo sulfide-support and improvement the sulfidation degree NiMoV/Al2O3-Ga2O3(SG) as showed sulfur analysis CHONS. The largest proportion of AlO4 content using the impregnation method to add Ga was verified by 27Al solid-state MAS NMR. The EDS elemental mapping confirmed that Ni, Mo, Al, Ga, V and S are well-distributed on support. The HRTEM analysis shows that the length and stacking distribution of MoS2 crystallites varied from 5.67 to 6.01 nm and 2.46 to 2.74 when using the sol–gel and impregnation synthesis method, respectively. The catalytic results revealed that the synthesis method induced the presence of gallium on the surface influencing the dispersion V5+ species, whose effect could have some relation with strength and density of acid sites that in turn influence the dispersion of the MoS2 phase, which correlates well with the indole HDN activities. The activities as indole HDN pseudo-first-order rate constants’ values (kHDN) from 0.29 to 2.78 mol/(m2·h): NiMoV/Al2O3 < NiMoV/Al2O3-Ga2O3(I) < NiMo/Al2O3 < NiMoV/Al2O3-Ga2O3(SG). Nevertheless, the nature of the active site can be related with reaction pathways, that is, NiMoV/Al2O3-Ga2O3(SG) and NiMoV/Al2O3-Ga2O3(I) catalysts produce ECH through HIND, while NiMoV/Al2O3 and NiMo/Al2O3 produce EB by hydrogenolysis of HIND to OEA. In the regard, the Ga and V act as structural promoters in the NiMo catalysts, allowing the largest generation of NiMoS M-edge-like and BRIM sites for HDN.Puello-Polo, EsneyderReales, Yelitce P.Marquez, EdgarLarruded, Dunieskys G.Costa Arzuza, Luis C.Toloza Toloza, Carlos-will be generated-orcid-0000-0003-3065-9693-600application/pdfengCorporación Universidad de la CostaCC0 1.0 Universalhttp://creativecommons.org/publicdomain/zero/1.0/info:eu-repo/semantics/openAccesshttp://purl.org/coar/access_right/c_abf2Catalysis Lettershttps://link.springer.com/article/10.1007/s10562-020-03438-yGalliumVanadiumModified al2O3Synthesis methodIndole hydrodenitrogenationEffect of gallium and vanadium in NiMoV/Al2O3-Ga2O3 catalysts on indole hydrodenitrogenationPre-Publicaciónhttp://purl.org/coar/resource_type/c_816bTextinfo:eu-repo/semantics/preprinthttp://purl.org/redcol/resource_type/ARTOTRinfo:eu-repo/semantics/acceptedVersionPublicationORIGINALEffect of Gallium and Vanadium.pdfEffect of Gallium and Vanadium.pdfapplication/pdf108468https://repositorio.cuc.edu.co/bitstreams/cd45dd51-1829-4d70-bcdc-4cfc7983f428/download43a1353426cb8ea0dbe5a3512d71edcbMD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8701https://repositorio.cuc.edu.co/bitstreams/d00ba395-7592-4070-97d0-8699ee4384e5/download42fd4ad1e89814f5e4a476b409eb708cMD52LICENSElicense.txtlicense.txttext/plain; charset=utf-83196https://repositorio.cuc.edu.co/bitstreams/a7e2e629-f6d6-4423-8709-d5d68f2dfc6d/downloade30e9215131d99561d40d6b0abbe9badMD53THUMBNAILEffect of Gallium and Vanadium.pdf.jpgEffect of Gallium and Vanadium.pdf.jpgimage/jpeg68233https://repositorio.cuc.edu.co/bitstreams/672a583d-35ab-4238-8202-0e32197d094f/downloadedc9762d6dcd481285101008287a3d4dMD54TEXTEffect of Gallium and Vanadium.pdf.txtEffect of Gallium and 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