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Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels

dc.contributor.authorRibeiro, Susana
dc.contributor.authorAlmeida, Pedro L.
dc.contributor.authorPires, João
dc.contributor.authorDe Castro, Baltazar
dc.contributor.authorBalula, Salete
dc.date.accessioned2020-06-17T14:18:54Z
dc.date.available2020-06-17T14:18:54Z
dc.date.issued2020-08-01
dc.description.abstractNovel material catalysts based in the active zinc-substituted polyoxotungstate ([PW11Zn(H2O)(39)](5-), abbreviated as PW11Zn) were efficiently used in the oxidative desulfurization of real and model diesels. These active catalytic center was strategically immobilized in a less hydrophilic periodic mesoporous organosilicas (PMOs), containing ethane-bridge (PMOE) and benzene-bridge (PMOB) walls, functionalized with (3-aminopropyl)triethoxysilane (aptes). The efficiency of the novel catalytic composites (PW11Zn@aptesPMOE and PM11Zn@aptesPMOB) was studied under oxidative desulfurization system (CODS) without the presence of an extraction solvent and also using a biphasic (diesel/extraction solvent) oxidative desulfurization system (ECODS). Both composites presented higher desulfurization efficiency under the solvent-free system, reaching ultra-low levels of sulfur compounds after only 1 h and using low ratio of H2O2/S = 4. The catalysts could be recycled without loss of activity for ten consecutive cycles. However, after the first desulfurization cycle complete desulfurization was achieved within only 30 min using PW11Zn@aptesPMOE composite. Also, the structure of PW it Zn@aptesPMOE demonstrated to be more stable than PW11Zn@aptesPMOB, probably due to the occurrence of some PW11Zn leaching from the PMOB surface, probably caused by the lower interaction of PW11Zn with the benzene-bridge PMOB wall. The most robust catalyst PW11Zn@aptesPMOE was used to desulfurize a real diesel achieving 75.9% of desulfurization after 2 h. The catalyst was further recycled with success to treat real diesel.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationRIBEIRO, Susana O.; [et al] – Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels. Microporous and Mesoporous Materials. ISSN 1387-1811. Vol. 302 (2020), pp. 1-11pt_PT
dc.identifier.doi10.1016/j.micromeso.2020.110193
dc.identifier.urihttp://hdl.handle.net/10400.21/11865
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relationUID/QUI/50006/2019 - project REQUIMTE-LAQVpt_PT
dc.relationPTDC/CTM-CTM/31983/2017 - project GlyGoldpt_PT
dc.relationUIDB/00100/2020 (CQE) - project GlyGoldpt_PT
dc.relationPOCI-01-0145-FEDER-007688 - national funds FCT/MECpt_PT
dc.relationADVANCED HETEROGENEOUS POROUS CATALYSTS FOR DESULFURIZATION OF DIESEL
dc.relation.publisherversionhttps://pdf.sciencedirectassets.com/271888/1-s2.0-S1387181120X00072/1-s2.0-S1387181120301967/main.pdf?X-Amz-Date=20200617T140633Z&X-Amz-Algorithm=AWS4-HMAC-SHA256&X-Amz-Signature=fe37f5a43c4902a3c6d9f3530e2fb07f9a19ef4ce5f86c320492f25490024c0c&X-Amz-Credential=ASIAQ3PHCVTYRFHCMUUS%2F20200617%2Fus-east-1%2Fs3%2Faws4_request&type=client&tid=prr-fd3410f3-25b2-4857-bb79-97c3a60d09f2&sid=859ce2df9726d342df7bc116edb764549f47gxrqb&pii=S1387181120301967&X-Amz-SignedHeaders=host&X-Amz-Security-Token=IQoJb3JpZ2luX2VjEF0aCXVzLWVhc3QtMSJHMEUCIQCFSNSd70BWXIe3%2BU0DMEpMvSCCy10PYcIVlh2reUqdoQIgVH2I%2BOrK4SkiM1Vi8Q3Y7BfT%2FEMgYPsa1LPaRu9gIvoqvQMI1v%2F%2F%2F%2F%2F%2F%2F%2F%2F%2FARADGgwwNTkwMDM1NDY4NjUiDE566ettQoRXUawAJCqRAw%2BPeKzWKwd3jYViF%2B8SmcLrcNpfgg%2FetCEE5FgHfHehuUxtoDR21H0IyKIakzhvky0x7Jao6wDsZKwHn5wkUzPeE%2FN8sNVO2Q02nFASuJAwZ%2FnPLgrBDmOG453ljV06cNp4kczwwy59fQzm%2Fm8PoHzPmMGe5HsxBXX7IMhdLfv6dKAG11KYH7DzluAOLPnfTaes9IKrtOq0%2FicrmtJx4ZdCCR9LrUIaulhCHOAhbTnigCYvOhH7L4GCZqN31t%2Fq0bS6tsGaU6daPhssPDr4fEdiCbXYEI4caMpKsl9WypN7j%2FLBo5c6vARz05kYJQ6PReq7wfCNgijO1uhcGeYBUilVRDeKKxvdwu%2FPDU0KMeq2aiLsmv7bM81Iw9eR4CEVx0IjZLg8pwSI6Jk4qSJ%2F4azK1owmsxuLXa7VQMryk54V3JdrgnuthR1p80LfhjYdqywgzqYLRRctRadTcq1%2BDHgskncT0CR195punN4vOHoLQ7FoGCKdbvGqdTnfxOIotVdqL26t1rGYJC9asUL8gIC4MIyiqPcFOusBTNdq604e4UA8y0%2BpBpQtidiBb5EqP3039ZoFXZKZJ6CQu7p7s%2FoAoXMyeYgXd%2FprWuppIvhVvTqe5HaoH39CqgLvc%2Bq%2BbwZeUaB8vmR19kSgxXQw14zsOMB37W7rlBDkQCnN1H8EeoZ4Jzkri%2BZnQ2EOOf4fvDQyUBiHlwYQk%2FjxFztZQAshQ22%2FmcVRCYVxdPs%2B2uIXRSyR3tsAbVskWQQU6t1k2r8qhW13zgbNAlf%2BI7ACiAEw3n9HymFhhHzjjVI69Fly44dCAUnqUWkqh6yQMQ2YpfYRLj2xhkjUT99mxxUdEF8bLj25oQ%3D%3D&host=68042c943591013ac2b2430a89b270f6af2c76d8dfd086a07176afe7c76c2c61&X-Amz-Expires=300&hash=766a76924698ae9a58ebd5be0a3e8dafd26e1cdf5d4b689ccd6af340495cd285pt_PT
dc.subjectMesoporous organosilicapt_PT
dc.subjectOxidative desulfurizationpt_PT
dc.subjectHydrogen peroxidept_PT
dc.subjectPolyoxometalatept_PT
dc.subjectReal dieselpt_PT
dc.subjectModel dieselpt_PT
dc.titlePolyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of dieselspt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardTitleADVANCED HETEROGENEOUS POROUS CATALYSTS FOR DESULFURIZATION OF DIESEL
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FCTM%2F50025%2F2013/PT
oaire.awardURIinfo:eu-repo/grantAgreement/FCT//SFRH%2FBD%2F95571%2F2013/PT
oaire.citation.endPage11pt_PT
oaire.citation.startPage1pt_PT
oaire.citation.titleMicroporous and Mesoporous Materialspt_PT
oaire.citation.volume302pt_PT
oaire.fundingStream5876
person.familyNameRibeiro
person.familyNameMarques de Almeida
person.familyNamePires
person.familyNamede Castro
person.familyNameBalula
person.givenNameSusana
person.givenNamePedro
person.givenNameJoão
person.givenNameBaltazar
person.givenNameSalete
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project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
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