Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts
Autor(a) principal: | |
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Data de Publicação: | 2018 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1016/j.apcata.2018.03.020 http://hdl.handle.net/11449/160319 |
Resumo: | Investigation was made on the effect of chromium content, and method of hydrothermal preparation of Cr/ZrO2 catalysts on their catalytic properties for CO2 oxidative dehydrogenation of propane (ODP). The catalysts were characterized by nitrogen physisorption, X-ray diffraction, Raman spectroscopy, and temperature programmed reduction and desorption of CO2 (TPD-CO2). The Cr/ZrO2 catalysts containing various chromium contents between 2.5 and 15 wt.% of Cr were prepared by conventional and microwave-assisted hydrothermal methods. Tetragonal ZrO2 was formed, with higher Cr contents, and smaller crystallite sizes obtained using the microwave -assisted method. The relationship between selectivity to propene and propane conversion suggested that independent of the preparation method, the catalytic properties could be classified in two groups, with low and high chromium contents. The TPD-CO2 results showed that a fraction of the CO2 was desorbed at temperatures higher than 500 degrees C, with simultaneous reduction of Cr(VI) species. The presence of CO2 in the reactants caused strong decreases of activity, selectivity, and yield towards propene. These results suggested that CO2 adsorbed strongly on the chromium oxide active sites for dehydrogenation of propane. The Cr/ZrO2 catalysts were active and selective for dehydrogenation of propane in the absence of CO2 (CDP), and became deactivated with time on stream. The activity was reestablished by thermal treatment with CO2 or O-2 after deactivation in CDP catalytic cycles, with the activity always being reestablished by treatment in O-2. The deactivation occurred by reduction of Cr(VI) species and by deposition of carbonaceous species produced in oligomerization reactions. |
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Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalystsChromium-zirconium oxidesMicrowaveOxidative dehydrogenation of propaneCO2Basic sitesInvestigation was made on the effect of chromium content, and method of hydrothermal preparation of Cr/ZrO2 catalysts on their catalytic properties for CO2 oxidative dehydrogenation of propane (ODP). The catalysts were characterized by nitrogen physisorption, X-ray diffraction, Raman spectroscopy, and temperature programmed reduction and desorption of CO2 (TPD-CO2). The Cr/ZrO2 catalysts containing various chromium contents between 2.5 and 15 wt.% of Cr were prepared by conventional and microwave-assisted hydrothermal methods. Tetragonal ZrO2 was formed, with higher Cr contents, and smaller crystallite sizes obtained using the microwave -assisted method. The relationship between selectivity to propene and propane conversion suggested that independent of the preparation method, the catalytic properties could be classified in two groups, with low and high chromium contents. The TPD-CO2 results showed that a fraction of the CO2 was desorbed at temperatures higher than 500 degrees C, with simultaneous reduction of Cr(VI) species. The presence of CO2 in the reactants caused strong decreases of activity, selectivity, and yield towards propene. These results suggested that CO2 adsorbed strongly on the chromium oxide active sites for dehydrogenation of propane. The Cr/ZrO2 catalysts were active and selective for dehydrogenation of propane in the absence of CO2 (CDP), and became deactivated with time on stream. The activity was reestablished by thermal treatment with CO2 or O-2 after deactivation in CDP catalytic cycles, with the activity always being reestablished by treatment in O-2. The deactivation occurred by reduction of Cr(VI) species and by deposition of carbonaceous species produced in oligomerization reactions.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)DEQ UFSCar, Rodovia Washington Luis,Km 235, Sao Carlos, SP, BrazilIBILCE UNESP, Rua Cristovao Colombo 2265, Sao Jose Do Rio Preto, SP, BrazilIBILCE UNESP, Rua Cristovao Colombo 2265, Sao Jose Do Rio Preto, SP, BrazilElsevier B.V.Universidade Federal de São Carlos (UFSCar)Universidade Estadual Paulista (Unesp)Oliveira, Joao F. S. deVolanti, Diogo P. [UNESP]Bueno, Jose M. C.Ferreira, Adriana P.2018-11-26T16:01:22Z2018-11-26T16:01:22Z2018-05-25info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article55-66application/pdfhttp://dx.doi.org/10.1016/j.apcata.2018.03.020Applied Catalysis A-general. Amsterdam: Elsevier Science Bv, v. 558, p. 55-66, 2018.0926-860Xhttp://hdl.handle.net/11449/16031910.1016/j.apcata.2018.03.020WOS:000433269700007WOS000433269700007.pdf23547399804067250000-0001-9315-9392Web of Sciencereponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengApplied Catalysis A-generalinfo:eu-repo/semantics/openAccess2023-09-30T06:03:48Zoai:repositorio.unesp.br:11449/160319Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462023-09-30T06:03:48Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
title |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
spellingShingle |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts Oliveira, Joao F. S. de Chromium-zirconium oxides Microwave Oxidative dehydrogenation of propane CO2 Basic sites |
title_short |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
title_full |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
title_fullStr |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
title_full_unstemmed |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
title_sort |
Effect of CO2 in the oxidative dehydrogenation reaction of propane over Cr/ZrO2 catalysts |
author |
Oliveira, Joao F. S. de |
author_facet |
Oliveira, Joao F. S. de Volanti, Diogo P. [UNESP] Bueno, Jose M. C. Ferreira, Adriana P. |
author_role |
author |
author2 |
Volanti, Diogo P. [UNESP] Bueno, Jose M. C. Ferreira, Adriana P. |
author2_role |
author author author |
dc.contributor.none.fl_str_mv |
Universidade Federal de São Carlos (UFSCar) Universidade Estadual Paulista (Unesp) |
dc.contributor.author.fl_str_mv |
Oliveira, Joao F. S. de Volanti, Diogo P. [UNESP] Bueno, Jose M. C. Ferreira, Adriana P. |
dc.subject.por.fl_str_mv |
Chromium-zirconium oxides Microwave Oxidative dehydrogenation of propane CO2 Basic sites |
topic |
Chromium-zirconium oxides Microwave Oxidative dehydrogenation of propane CO2 Basic sites |
description |
Investigation was made on the effect of chromium content, and method of hydrothermal preparation of Cr/ZrO2 catalysts on their catalytic properties for CO2 oxidative dehydrogenation of propane (ODP). The catalysts were characterized by nitrogen physisorption, X-ray diffraction, Raman spectroscopy, and temperature programmed reduction and desorption of CO2 (TPD-CO2). The Cr/ZrO2 catalysts containing various chromium contents between 2.5 and 15 wt.% of Cr were prepared by conventional and microwave-assisted hydrothermal methods. Tetragonal ZrO2 was formed, with higher Cr contents, and smaller crystallite sizes obtained using the microwave -assisted method. The relationship between selectivity to propene and propane conversion suggested that independent of the preparation method, the catalytic properties could be classified in two groups, with low and high chromium contents. The TPD-CO2 results showed that a fraction of the CO2 was desorbed at temperatures higher than 500 degrees C, with simultaneous reduction of Cr(VI) species. The presence of CO2 in the reactants caused strong decreases of activity, selectivity, and yield towards propene. These results suggested that CO2 adsorbed strongly on the chromium oxide active sites for dehydrogenation of propane. The Cr/ZrO2 catalysts were active and selective for dehydrogenation of propane in the absence of CO2 (CDP), and became deactivated with time on stream. The activity was reestablished by thermal treatment with CO2 or O-2 after deactivation in CDP catalytic cycles, with the activity always being reestablished by treatment in O-2. The deactivation occurred by reduction of Cr(VI) species and by deposition of carbonaceous species produced in oligomerization reactions. |
publishDate |
2018 |
dc.date.none.fl_str_mv |
2018-11-26T16:01:22Z 2018-11-26T16:01:22Z 2018-05-25 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1016/j.apcata.2018.03.020 Applied Catalysis A-general. Amsterdam: Elsevier Science Bv, v. 558, p. 55-66, 2018. 0926-860X http://hdl.handle.net/11449/160319 10.1016/j.apcata.2018.03.020 WOS:000433269700007 WOS000433269700007.pdf 2354739980406725 0000-0001-9315-9392 |
url |
http://dx.doi.org/10.1016/j.apcata.2018.03.020 http://hdl.handle.net/11449/160319 |
identifier_str_mv |
Applied Catalysis A-general. Amsterdam: Elsevier Science Bv, v. 558, p. 55-66, 2018. 0926-860X 10.1016/j.apcata.2018.03.020 WOS:000433269700007 WOS000433269700007.pdf 2354739980406725 0000-0001-9315-9392 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Applied Catalysis A-general |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
55-66 application/pdf |
dc.publisher.none.fl_str_mv |
Elsevier B.V. |
publisher.none.fl_str_mv |
Elsevier B.V. |
dc.source.none.fl_str_mv |
Web of Science reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
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1799964375845437440 |