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dc.contributor.advisorKuhn, Alexander
dc.contributor.advisorLimtrakul, Jumras
dc.contributor.authorWATTANAKIT, Chularat
dc.contributor.otherWarakulwit, Chompunuch
dc.date2013-08-06
dc.date.accessioned2020-12-14T21:16:24Z
dc.date.available2020-12-14T21:16:24Z
dc.identifier.urihttp://ori-oai.u-bordeaux1.fr/pdf/2013/WATTANAKIT_CHULARAT_2013.pdf
dc.identifier.urihttps://tel.archives-ouvertes.fr/tel-00912339
dc.identifier.urihttps://oskar-bordeaux.fr/handle/20.500.12278/22594
dc.identifier.nnt2013BOR14819
dc.description.abstractDans ce travail nous étudions l’élaboration, la caractérisation et les applications de différents matériaux poreux. L’étude est organisée en trois parties majeures: la synthèse de zéolithes micro/mesoporeux et leur application potentielle dans l’industrie pétrochimique, l’étude théorique de mécanismes réactionnels sur des zeolites microporeux, et le design de métaux mesoporeux avec une chiralité intrinsèque de leur surface interne. Ces matériaux poreux montrent des propriétés excellentes, notamment pour des applications potentielles en catalyse et comme interfaces chirales.
dc.description.abstractEnIn the present work, the elaboration, characterisation and applications of differentporous materials have been studied. Porous materials are divided into three categoriesdepending on the porous cavity size, namely microporous materials (pore diameter < 2nm), mesoporous materials (2 nm < pore diameter < 50 nm) and macroporous materials(pore diameter > 50 nm). The thesis work is organized in three major parts: the synthesisof hierarchical micro/mesoporous zeolites and their potential application for thepetrochemical industry, the theoretical study of reaction mechanisms on microporouszeolite and the design of mesoporous metals with intrinsic chirality at their inner surface.The hierarchical micro/mesoporous zeolite, composed of microporous andmesoporous features, has been prepared using carbon-silica (C/SiO2) composites derivedfrom a pyrolysis of hydrocarbon gas on silica gel. Our findings demonstrate that not onlythe presence of a high surface area and porosity, but also an improved efficiency of thesematerials for many petrochemical processes such as n-butene isomerization, nhexadecanecatalytic cracking and hydrocracking. The novel synthetic method is expectedto be generalized for other types of zeolites, and is considered to be a promising methodfor creating hierarchical micro/mesoporous zeolites for potential catalytic applications,especially in the petrochemical industry.In addition to the study of practical catalytic aspects, a theoretical approach hasbeen used to investigate potential reaction mechanisms such as the selective isomerizationof 1-butene into isobutene. More specifically, the monomolecular skeletal isomerizationof 1-butene into isobutene on H-FER zeolite was theoretically studied by using theONIOM approach. This process was found to involve the transformation of adsorbed 1-butene through 2-butoxide, isobutoxide, and tert-butyl cation intermediates. The ratedeterminingstep is the conversion of isobutoxide into isobutene, in which the reactionhas to proceed through the primary isobutyl cation transition state. The shape selectivitydue to the “nano-confinement” effect of the zeolite framework strongly affects theadsorption, the stability of alkoxide species and carbenium ion, as well as the skeletalisomerization mechanism of 1-butene.Moreover, the microporous and mesoporous zeolite, the generation of chiralmesoporous metal and its enantioselective recognition properties have been studied.Molecular imprinting (MI) is a major approach for generating materials withenantioselective properties. In this work, a chiral imprinted mesoporous platinum hasbeen obtained by the electrochemical reduction of platinum salts in the simultaneouspresence of a lyotropic liquid crystal phase and chiral template molecules. The resultingmaterials exhibit not only a dramatic increase in active surface area due to theirmesoporosity, but also a significant discrimination between two enantiomers of a chiralprobe, confirmed by both electrochemical and enantioselective adsorption experiments.Most importantly the porous platinum retains its chiral character even after removal of thechiral template molecule. Our findings could lead to the development of new materials,which are of potential interest for applications in areas such as chiral synthesis, sensors,separation, purification and drug development.
dc.language.isoen
dc.subjectZéolithes micro- et mesoporeux
dc.subjectCatalyseurs
dc.subjectMétaux mesoporeux chiraux
dc.subjectÉlectroanalyse
dc.subjectCalcul quantique
dc.subject.enHierarchical micro/mesoprorous zeolite
dc.subject.enSkeletal isomerization
dc.subject.enCatalysts
dc.subject.enNano-confinement
dc.subject.enChiral mesoporous metal
dc.subject.enLyotropic liquid crystal
dc.subject.enElectrodeposition
dc.subject.enElectroanalysis
dc.titleÉlaboration et application de matériaux poreux : études théoriques et expérimentales
dc.title.enThe novel synthesis of microporous and mesoporous materials and their applications for hydrocarbon transformation and chiral recognition
dc.typeThèses de doctorat
dc.contributor.jurypresidentBopp, Philippe
bordeaux.hal.laboratoriesThèses de l'Université de Bordeaux avant 2014*
bordeaux.hal.laboratoriesInstitut des Sciences Moléculaires (Bordeaux)
bordeaux.hal.laboratoriesInstitut des Sciences Moléculaires / ISM
bordeaux.institutionUniversité de Bordeaux
bordeaux.type.institutionBordeaux 1
bordeaux.thesis.disciplineChimie-physique
bordeaux.ecole.doctoraleÉcole doctorale des sciences chimiques (Talence, Gironde)
star.origin.linkhttps://www.theses.fr/2013BOR14819
dc.contributor.rapporteurSchulte, Albert
dc.contributor.rapporteurJongsomjit, Bumjerd
bordeaux.COinSctx_ver=Z39.88-2004&amp;rft_val_fmt=info:ofi/fmt:kev:mtx:journal&amp;rft.title=%C3%89laboration%20et%20application%20de%20mat%C3%A9riaux%20poreux%20:%20%C3%A9tudes%20th%C3%A9oriques%20et%20exp%C3%A9rimentales&amp;rft.atitle=%C3%89laboration%20et%20application%20de%20mat%C3%A9riaux%20poreux%20:%20%C3%A9tudes%20th%C3%A9oriques%20et%20exp%C3%A9rimentales&amp;rft.au=WATTANAKIT,%20Chularat&amp;rft.genre=unknown


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