Publicação
Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity
| Resumo: | A bentonite collected at Serra de Dentro (SD), Porto Santo Island, Portugal, and the source clay SAz-1 (Cheto, Arizona) were ion-exchanged with different cations (Al3+, Ni2+, Cr3+ and Na+ ). Variable temperature diffuse reflectance infrared Fourier transform spectroscopy (VT-DRIFTS) of pyridine treated samples, thermal desorption of cyclohexylamine and real time mass spectrometry of the evolved gases were used to evaluate the acidic properties of the prepared catalysts. The catalytic activity of these ion-exchanged clays was tested in the acid-catalysed conversion of limonene at 150 8C, to yield isomerization products (terpinolene, a-terpinene, g-terpinene and isoterpinolene), disproportionation products ( p cymene and p-menthenes) and high molecular-weight compounds. The possibility of increasing the selectivity toward p-cymene, over a catalyst with substantial Lewis acid character, was particularly envisaged. Catalysts derived from SD were significantly more active than their SAz-1 counterparts. This was mainly attributed to the greater inherent acidity, to the higher structural iron content (providing dehydrogenation activity) and to the higher nitrogen surface area of the starting SD clays. Within the Mn+ -SD series, the order of activity decreased as Ni2+ > Al3+ > Cr3+ > Na+ . A direct comparison between Al3+-SD (with maximized Bro¨nsted acidity) and Ni2+-SD (with predominant Lewis acid character) provided no support for enhanced p-cymene production over Lewis acid sites. |
|---|---|
| Autores principais: | Catrinescu, C. |
| Outros Autores: | Fernandes, César; Castilho, P.; Breen, C. |
| Assunto: | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| Ano: | 2006 |
| País: | Portugal |
| Tipo de documento: | artigo |
| Tipo de acesso: | acesso aberto |
| Instituição associada: | Universidade da Madeira |
| Idioma: | inglês |
| Origem: | DigitUMa - Repositório da Universidade da Madeira |
| _version_ | 1877781927773077504 |
|---|---|
| author | Catrinescu, C. |
| author2 | Fernandes, César Castilho, P. Breen, C. |
| author2_role | author author author |
| author_facet | Catrinescu, C. Fernandes, César Castilho, P. Breen, C. |
| author_role | author |
| contributor_name_str_mv | DigitUMa |
| country_str | PT |
| creators_json_txt | [{\"Person.name\":\"Catrinescu, C.\"},{\"Person.name\":\"Fernandes, César\",\"Person.identifier.orcid\":\"0000-0001-9289-9962\",\"Person.identifier.scopusAuthorID\":\"14064572200\"},{\"Person.name\":\"Castilho, P.\",\"Person.identifier.cienciaID\":\"6D15-8C69-A2E0\",\"Person.identifier.orcid\":\"0000-0002-8303-4286\"},{\"Person.name\":\"Breen, C.\"}] |
| datacite.contributors.contributor.contributorName.fl_str_mv | DigitUMa |
| datacite.creators.creator.creatorName.fl_str_mv | Catrinescu, C. Fernandes, César Castilho, P. Breen, C. |
| datacite.date.Accepted.fl_str_mv | 2006-01-01T00:00:00Z |
| datacite.date.available.fl_str_mv | 2021-04-09T11:22:04Z |
| datacite.date.embargoed.fl_str_mv | 2021-04-09T11:22:04Z |
| datacite.rights.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| datacite.subjects.subject.fl_str_mv | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| datacite.titles.title.fl_str_mv | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| dc.contributor.none.fl_str_mv | DigitUMa |
| dc.creator.none.fl_str_mv | Catrinescu, C. Fernandes, César Castilho, P. Breen, C. |
| dc.date.Accepted.fl_str_mv | 2006-01-01T00:00:00Z |
| dc.date.available.fl_str_mv | 2021-04-09T11:22:04Z |
| dc.date.embargoed.fl_str_mv | 2021-04-09T11:22:04Z |
| dc.format.none.fl_str_mv | application/pdf |
| dc.identifier.none.fl_str_mv | http://hdl.handle.net/10400.13/3268 |
| dc.language.none.fl_str_mv | eng |
| dc.publisher.none.fl_str_mv | Elsevier |
| dc.rights.cclincense.fl_str_mv | http://creativecommons.org/licenses/by/4.0/ |
| dc.rights.none.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| dc.subject.none.fl_str_mv | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| dc.title.fl_str_mv | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| dc.type.none.fl_str_mv | http://purl.org/coar/resource_type/c_6501 |
| description | A bentonite collected at Serra de Dentro (SD), Porto Santo Island, Portugal, and the source clay SAz-1 (Cheto, Arizona) were ion-exchanged with different cations (Al3+, Ni2+, Cr3+ and Na+ ). Variable temperature diffuse reflectance infrared Fourier transform spectroscopy (VT-DRIFTS) of pyridine treated samples, thermal desorption of cyclohexylamine and real time mass spectrometry of the evolved gases were used to evaluate the acidic properties of the prepared catalysts. The catalytic activity of these ion-exchanged clays was tested in the acid-catalysed conversion of limonene at 150 8C, to yield isomerization products (terpinolene, a-terpinene, g-terpinene and isoterpinolene), disproportionation products ( p cymene and p-menthenes) and high molecular-weight compounds. The possibility of increasing the selectivity toward p-cymene, over a catalyst with substantial Lewis acid character, was particularly envisaged. Catalysts derived from SD were significantly more active than their SAz-1 counterparts. This was mainly attributed to the greater inherent acidity, to the higher structural iron content (providing dehydrogenation activity) and to the higher nitrogen surface area of the starting SD clays. Within the Mn+ -SD series, the order of activity decreased as Ni2+ > Al3+ > Cr3+ > Na+ . A direct comparison between Al3+-SD (with maximized Bro¨nsted acidity) and Ni2+-SD (with predominant Lewis acid character) provided no support for enhanced p-cymene production over Lewis acid sites. |
| dirty | 0 |
| eu_rights_str_mv | openAccess |
| format | article |
| fulltext.url.fl_str_mv | https://digituma.uma.pt/bitstreams/fa69abf4-3fc5-4430-8ccc-64b1f8abde9c/download |
| funder_facet_str_mv | FCT{{{_:::_}}}Fundação para a Ciência e a Tecnologia |
| 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 |
| funding.identifier_str_mv | POCTI/CTM/47619/2002 |
| funding.name_str_mv | POCI |
| funding_str_mv | POCTI/CTM/47619/2002 info:eu-repo/grantAgreement/FCT/POCI/POCTI%2FCTM%2F47619%2F2002/PT |
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| identifier.url.fl_str_mv | http://hdl.handle.net/10400.13/3268 |
| inst_facet_str | urn:organizationAcronym:digituma{{{_:::_}}}Universidade da Madeira |
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| institution | Universidade da Madeira |
| instname_str | Universidade da Madeira |
| language | eng |
| network_acronym_str | digituma |
| network_name_str | DigitUMa - Repositório da Universidade da Madeira |
| oai_identifier_str | oai:digituma.uma.pt:10400.13/3268 |
| organization_str_mv | urn:organizationAcronym:digituma |
| person_str_mv | Catrinescu, C. Fernandes, César Fernandes, César http://orcid.org/0000-0001-9289-9962 0000-0001-9289-9962 Castilho, P. Castilho, P. https://www.ciencia-id.pt/6D15-8C69-A2E0 6D15-8C69-A2E0 http://orcid.org/0000-0002-8303-4286 0000-0002-8303-4286 Breen, C. |
| publishDate | 2006 |
| publisher.none.fl_str_mv | Elsevier |
| repo_facet_str | urn:repositoryAcronym:digituma{{{_:::_}}}DigitUMa - Repositório da Universidade da Madeira |
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| spelling | engElsevierpt_PTA bentonite collected at Serra de Dentro (SD), Porto Santo Island, Portugal, and the source clay SAz-1 (Cheto, Arizona) were ion-exchanged with different cations (Al3+, Ni2+, Cr3+ and Na+ ). Variable temperature diffuse reflectance infrared Fourier transform spectroscopy (VT-DRIFTS) of pyridine treated samples, thermal desorption of cyclohexylamine and real time mass spectrometry of the evolved gases were used to evaluate the acidic properties of the prepared catalysts. The catalytic activity of these ion-exchanged clays was tested in the acid-catalysed conversion of limonene at 150 8C, to yield isomerization products (terpinolene, a-terpinene, g-terpinene and isoterpinolene), disproportionation products ( p cymene and p-menthenes) and high molecular-weight compounds. The possibility of increasing the selectivity toward p-cymene, over a catalyst with substantial Lewis acid character, was particularly envisaged. Catalysts derived from SD were significantly more active than their SAz-1 counterparts. This was mainly attributed to the greater inherent acidity, to the higher structural iron content (providing dehydrogenation activity) and to the higher nitrogen surface area of the starting SD clays. Within the Mn+ -SD series, the order of activity decreased as Ni2+ > Al3+ > Cr3+ > Na+ . A direct comparison between Al3+-SD (with maximized Bro¨nsted acidity) and Ni2+-SD (with predominant Lewis acid character) provided no support for enhanced p-cymene production over Lewis acid sites.application/pdfpt_PTInfluence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivityCatrinescu, C.PersonalFernandes, CésarDSpacehttp://dspace.org/items/482857a3-4e6d-4453-bfc1-afb17ff8ce2aDSpacehttp://dspace.org/items/482857a3-4e6d-4453-bfc1-afb17ff8ce2aFernandesCesarORCIDhttp://orcid.org0000-0001-9289-9962Scopus Author IDhttps://www.scopus.com14064572200PersonalCastilho, P.DSpacehttp://dspace.org/items/d84fd917-438e-43bf-ac6f-256562481c05DSpacehttp://dspace.org/items/d84fd917-438e-43bf-ac6f-256562481c05CastilhoPaula CCiência IDhttps://www.ciencia-id.pt6D15-8C69-A2E0ORCIDhttp://orcid.org0000-0002-8303-4286Breen, C.HostingInstitutionOrganizationalDigitUMae-mailmailto:digituma@uma.ptdigituma@uma.ptDOIIsPartOf10.1016/j.apcata.2006.06.0232021-04-09T11:22:04Z20062006-01-01T00:00:00ZHandlehttp://hdl.handle.net/10400.13/3268http://purl.org/coar/access_right/c_abf2open accessIon-exchanged claysAcidityCatalysisLimonenep-Cymene.Faculdade de Ciências Exatas e da Engenharia496451 bytesFundação para a Ciência e a TecnologiaCLAYCATS - Modified Porto Santo Clays as catalysts for liquid phase organic reactionsinfo:eu-repo/grantAgreement/FCT/POCI/POCTI%2FCTM%2F47619%2F2002/PTPOCTI/CTM/47619/2002POCICrossref Funder IDhttp://doi.org/10.13039/501100001871literaturehttp://purl.org/coar/resource_type/c_6501journal article2006http://creativecommons.org/licenses/by/4.0/http://purl.org/coar/access_right/c_abf2application/pdffulltexthttps://digituma.uma.pt/bitstreams/fa69abf4-3fc5-4430-8ccc-64b1f8abde9c/downloadApplied Catalysis A: General311172184 |
| spellingShingle | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity Catrinescu, C. Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| status | SINGLETON |
| subject.fl_str_mv | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| title | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| title_full | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| title_fullStr | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| title_full_unstemmed | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| title_short | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| title_sort | Influence of exchange cations on the catalytic conversion of limonene over Serra de Dentro (SD) and SAz-1 clays: correlations between acidity and catalytic activity/selectivity |
| topic | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| topic_facet | Ion-exchanged clays Acidity Catalysis Limonene p-Cymene . Faculdade de Ciências Exatas e da Engenharia |
| url | http://hdl.handle.net/10400.13/3268 |
| visible | 1 |