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Oxidative desulfurization strategies using Keggin-type polyoxometalate catalysts: Biphasic versus solvent-free systems

2019-08-01Journal article Restricted access
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dc.contributor.authorRibeiro, Susana
dc.contributor.authorGranadeiro, Carlos
dc.contributor.authorAlmeida, Pedro L.
dc.contributor.authorPires, João
dc.contributor.authorCapel-Sanchez, Maria C.
dc.contributor.authorCampos-Martin, J. M.
dc.contributor.authorGago, S.
dc.contributor.authorDe Castro, Baltazar
dc.contributor.authorBalula, Salete
dc.date.accessioned2019-07-19T09:31:18Z
dc.date.available2019-07-19T09:31:18Z
dc.date.issued2019-08-01
dc.description.abstractStrategic polyoxometalate Keggin-type structural modification was performed to increase the oxidative catalytic performance to desulfurize model and real diesels. The most active lacunar structure [PW11O39](7-) (PW11) showed to complete desulfurize a simulated diesel after 60 min at 70 degrees C. Its application as homogeneous catalyst using a biphasic system 1: 1 diesel/acetonitrile needed to use an excess of oxidant (ratio H2O2/S = 8). The immobilization of the PW11 on amine-functionalized SBA-15 supports originated two heterogeneous catalysts PW11@aptesSBA-15 and PW11@tbaSBA-15. The best results were attained with the PW11@aptesSBA-15 catalyst showing identical oxidative desulfurization performance as the homogeneous analogue. As advantage, this heterogeneous catalyst promotes the complete desulfurization of simulated diesel using a solvent-free system, i.e. without the need of acetonitrile use. On the other hand, the same desulfurization efficiency could be achieved using half the amount of oxidant (H2O2/S = 4). The oxidative desulfurization of the real diesel achieved a remarkable 83.4% of efficiency after just 2 h. The recycling capacity of PW11@aptesSBA-15 catalyst was confirmed for eight consecutive cycles using the biphasic and the solvent-free systems. Its stability investigation demonstrates to be higher under the solvent-free system than the biphasic system, without practically any occurrence of PW11 leaching in the first case. On the other hand, the Venturello peroxocomplex [PO4{W(O-2)(2)}(4)](3-), recognized as active intermediate in the homogeneous biphasic system, was not identified in the heterogeneous catalytic systems.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationRIBEIRO, Susana O.; [et al] – Oxidative desulfurization strategies using Keggin-type polyoxometalate catalysts: Biphasic versus solvent-free systems. Catalysis Today. ISSN 0920-5861. Vol. 333, SI (2019), pp. 226-236pt_PT
dc.identifier.doi10.1016/j.cattod.2018.10.046pt_PT
dc.identifier.issn0920-5861
dc.identifier.issn1873-4308
dc.identifier.urihttp://hdl.handle.net/10400.21/10338
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relationPOCI-01-0145-FEDER-007265 - FCTpt_PT
dc.relationPOCI-01-0145-FEDER-007688 - FCTpt_PT
dc.relationADVANCED HETEROGENEOUS POROUS CATALYSTS FOR DESULFURIZATION OF DIESEL
dc.relationMULTIFUNCTIONAL COMPOSITE MATERIALS BASED IN POLYOXOMETALATES @ POROUS HYBRID SUPPORTS
dc.relation.publisherversionhttps://reader.elsevier.com/reader/sd/pii/S0920586118316468?token=D33C98610E9FD8B31CC8B19545656A7DA823F83DD3CA48AD2CFDEBAAB8FBFA0ACECE323A4A61C762CF811FA0ACBCA1ABpt_PT
dc.subjectOxidative desulfurizationpt_PT
dc.subjectReal dieselpt_PT
dc.subjectHeterogeneous catalysispt_PT
dc.subjectPolyoxotungstatespt_PT
dc.subjectHydrogen peroxidept_PT
dc.titleOxidative desulfurization strategies using Keggin-type polyoxometalate catalysts: Biphasic versus solvent-free systemspt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardTitleADVANCED HETEROGENEOUS POROUS CATALYSTS FOR DESULFURIZATION OF DIESEL
oaire.awardTitleMULTIFUNCTIONAL COMPOSITE MATERIALS BASED IN POLYOXOMETALATES @ POROUS HYBRID SUPPORTS
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FQUI%2F50006%2F2013/PT
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oaire.awardURIinfo:eu-repo/grantAgreement/FCT//SFRH%2FBD%2F95571%2F2013/PT
oaire.awardURIinfo:eu-repo/grantAgreement/FCT//SFRH%2FBPD%2F73191%2F2010/PT
oaire.citation.endPage236pt_PT
oaire.citation.startPage226pt_PT
oaire.citation.titleCatalysis Todaypt_PT
oaire.citation.volume333pt_PT
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person.givenNameCarlos
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person.givenNameJoão
person.givenNameJose M.
person.givenNameSandra
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rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
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