Publicação
Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels
| Resumo: | Novel 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. |
|---|---|
| Autores principais: | Ribeiro, Susana |
| Outros Autores: | Almeida, Pedro L.; Pires, João; De Castro, Baltazar; Balula, Salete |
| Assunto: | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| Ano: | 2020 |
| País: | Portugal |
| Tipo de documento: | artigo |
| Tipo de acesso: | acesso restrito |
| Instituição associada: | Instituto Politécnico de Lisboa |
| Idioma: | inglês |
| Origem: | Repositório Científico do Instituto Politécnico de Lisboa |
| _version_ | 1866887272937291776 |
|---|---|
| author | Ribeiro, Susana |
| author2 | Almeida, Pedro L. Pires, João De Castro, Baltazar Balula, Salete |
| author2_role | author author author author |
| author_facet | Ribeiro, Susana Almeida, Pedro L. Pires, João De Castro, Baltazar Balula, Salete |
| author_role | author |
| contributor_name_str_mv | RCIPL |
| country_str | PT |
| creators_json_txt | [{\"Person.name\":\"Ribeiro, Susana\",\"Person.identifier.orcid\":\"0000-0002-7402-9004\"},{\"Person.name\":\"Almeida, Pedro L.\",\"Person.identifier.orcid\":\"0000-0001-7356-8455\"},{\"Person.name\":\"Pires, João\",\"Person.identifier.orcid\":\"0000-0002-8374-558X\"},{\"Person.name\":\"De Castro, Baltazar\",\"Person.identifier.orcid\":\"0000-0001-9097-0171\"},{\"Person.name\":\"Balula, Salete\",\"Person.identifier.orcid\":\"0000-0002-8984-0473\"}] |
| datacite.contributors.contributor.contributorName.fl_str_mv | RCIPL |
| datacite.creators.creator.creatorName.fl_str_mv | Ribeiro, Susana Almeida, Pedro L. Pires, João De Castro, Baltazar Balula, Salete |
| datacite.date.Accepted.fl_str_mv | 2020-08-01T00:00:00Z |
| datacite.date.available.fl_str_mv | 2020-06-17T14:18:54Z |
| datacite.date.embargoed.fl_str_mv | 2020-06-17T14:18:54Z |
| datacite.rights.fl_str_mv | http://purl.org/coar/access_right/c_16ec |
| datacite.subjects.subject.fl_str_mv | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| datacite.titles.title.fl_str_mv | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| dc.contributor.none.fl_str_mv | RCIPL |
| dc.creator.none.fl_str_mv | Ribeiro, Susana Almeida, Pedro L. Pires, João De Castro, Baltazar Balula, Salete |
| dc.date.Accepted.fl_str_mv | 2020-08-01T00:00:00Z |
| dc.date.available.fl_str_mv | 2020-06-17T14:18:54Z |
| dc.date.embargoed.fl_str_mv | 2020-06-17T14:18:54Z |
| dc.format.none.fl_str_mv | application/pdf |
| dc.identifier.none.fl_str_mv | http://hdl.handle.net/10400.21/11865 |
| dc.language.none.fl_str_mv | eng |
| dc.publisher.none.fl_str_mv | Elsevier |
| dc.rights.none.fl_str_mv | http://purl.org/coar/access_right/c_16ec |
| dc.subject.none.fl_str_mv | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| dc.title.fl_str_mv | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| dc.type.none.fl_str_mv | http://purl.org/coar/resource_type/c_6501 |
| description | Novel 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. |
| dirty | 0 |
| eu_rights_str_mv | restrictedAccess |
| format | article |
| fulltext.url.fl_str_mv | https://repositorio.ipl.pt/bitstreams/2cab61ed-9cbf-4d05-9cc5-05823a2bdb33/download |
| funding.funder.alternateName_str_mv | FCT |
| funding.funder.identifier_str_mv | http://doi.org/10.13039/501100001871 |
| funding.funder.name_str_mv | Fundação para a Ciência e a Tecnologia |
| id | ripl_b2f7baf8bae935bdf32ef5ef6f8a321c |
| identifier.url.fl_str_mv | http://hdl.handle.net/10400.21/11865 |
| instacron_str | ipl |
| institution | Instituto Politécnico de Lisboa |
| instname_str | Instituto Politécnico de Lisboa |
| language | eng |
| network_acronym_str | ripl |
| network_name_str | Repositório Científico do Instituto Politécnico de Lisboa |
| oai_identifier_str | oai:repositorio.ipl.pt:10400.21/11865 |
| organization_str_mv | urn:organizationAcronym:ipl |
| person_str_mv | Ribeiro, Susana Ribeiro, Susana https://www.ciencia-id.pt/0E10-E54E-4314 0E10-E54E-4314 http://orcid.org/0000-0002-7402-9004 0000-0002-7402-9004 Almeida, Pedro L. Almeida, Pedro L. https://www.ciencia-id.pt/0218-71B2-2DE0 0218-71B2-2DE0 http://orcid.org/0000-0001-7356-8455 0000-0001-7356-8455 Pires, João Pires, João https://www.ciencia-id.pt/1014-6FC7-27CD 1014-6FC7-27CD http://orcid.org/0000-0002-8374-558X 0000-0002-8374-558X De Castro, Baltazar De Castro, Baltazar https://www.ciencia-id.pt/4D13-899F-862C 4D13-899F-862C http://orcid.org/0000-0001-9097-0171 0000-0001-9097-0171 Balula, Salete Balula, Salete https://www.ciencia-id.pt/E71B-9980-14F5 E71B-9980-14F5 http://orcid.org/0000-0002-8984-0473 0000-0002-8984-0473 |
| publishDate | 2020 |
| publisher.none.fl_str_mv | Elsevier |
| reponame_str | Repositório Científico do Instituto Politécnico de Lisboa |
| repository_id_str | urn:repositoryAcronym:ripl |
| service_str_mv | urn:repositoryAcronym:ripl |
| spelling | engElsevierpt_PTNovel 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.application/pdfpt_PTPolyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of dieselsPersonalRibeiro, SusanaDSpacehttp://dspace.org/items/4908380c-29a3-4dde-9a35-cca6e952f705DSpacehttp://dspace.org/items/4908380c-29a3-4dde-9a35-cca6e952f705RibeiroSusanaCiência IDhttps://www.ciencia-id.pt0E10-E54E-4314ORCIDhttp://orcid.org0000-0002-7402-9004Scopus Author IDhttps://www.scopus.com37100341000PersonalAlmeida, Pedro L.DSpacehttp://dspace.org/items/429b6d71-328e-42b3-8151-15493de249b8DSpacehttp://dspace.org/items/429b6d71-328e-42b3-8151-15493de249b8Marques de AlmeidaPedroCiência IDhttps://www.ciencia-id.pt0218-71B2-2DE0ORCIDhttp://orcid.org0000-0001-7356-8455Researcher IDhttps://www.researcherid.comB-4356-2009Scopus Author IDhttps://www.scopus.com57190384213PersonalPires, JoãoDSpacehttp://dspace.org/items/adfbda10-f00f-4ff1-8e3d-2ac8b6881e84DSpacehttp://dspace.org/items/adfbda10-f00f-4ff1-8e3d-2ac8b6881e84PiresJoãoCiência IDhttps://www.ciencia-id.pt1014-6FC7-27CDORCIDhttp://orcid.org0000-0002-8374-558XResearcher IDhttps://www.researcherid.comA-4155-2009Scopus Author IDhttps://www.scopus.com55960912300PersonalDe Castro, BaltazarDSpacehttp://dspace.org/items/7405ec49-115a-4b75-8cd6-228788dc6dceDSpacehttp://dspace.org/items/7405ec49-115a-4b75-8cd6-228788dc6dcede CastroBaltazarCiência IDhttps://www.ciencia-id.pt4D13-899F-862CORCIDhttp://orcid.org0000-0001-9097-0171Researcher IDhttps://www.researcherid.comD-8306-2013Scopus Author IDhttps://www.scopus.com7005254412PersonalBalula, SaleteDSpacehttp://dspace.org/items/d6f4ada6-de14-4147-9298-25e85d7241e8DSpacehttp://dspace.org/items/d6f4ada6-de14-4147-9298-25e85d7241e8BalulaSaleteCiência IDhttps://www.ciencia-id.ptE71B-9980-14F5ORCIDhttp://orcid.org0000-0002-8984-0473Scopus Author IDhttps://www.scopus.com16232273400HostingInstitutionOrganizationalRCIPLe-mailmailto:rcaap@sp.ipl.ptrcaap@sp.ipl.ptDOIIsPartOf10.1016/j.micromeso.2020.1101932020-06-17T14:18:54Z2020-08-012020-08-01T00:00:00ZHandlehttp://hdl.handle.net/10400.21/11865http://purl.org/coar/access_right/c_16ecrestricted accessMesoporous organosilicaOxidative desulfurizationHydrogen peroxidePolyoxometalateReal dieselModel diesel2553083 bytesFundação para a Ciência e a TecnologiaADVANCED HETEROGENEOUS POROUS CATALYSTS FOR DESULFURIZATION OF DIESELCrossref Funder IDhttp://doi.org/10.13039/501100001871literaturehttp://purl.org/coar/resource_type/c_6501journal articlehttp://purl.org/coar/access_right/c_16ecapplication/pdffulltexthttps://repositorio.ipl.pt/bitstreams/2cab61ed-9cbf-4d05-9cc5-05823a2bdb33/downloadMicroporous and Mesoporous Materials302111 |
| spellingShingle | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels Ribeiro, Susana Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| status | SINGLETON |
| subject.fl_str_mv | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| title | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| title_full | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| title_fullStr | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| title_full_unstemmed | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| title_short | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| title_sort | Polyoxometalate@Periodic mesoporous organosilicas as active materials for oxidative desulfurization of diesels |
| topic | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| topic_facet | Mesoporous organosilica Oxidative desulfurization Hydrogen peroxide Polyoxometalate Real diesel Model diesel |
| url | http://hdl.handle.net/10400.21/11865 |
| visible | 1 |