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Previous issue date: 2015-07-31 / Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico (CNPq) / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior (CAPES) / Os ligantes ?-diiminas 2-(fenil)amino-4-(fenil)imino-2-penteno e o 2-(2,6-dimetilfenil)amino-4-(2,6-dimetilfenil)imino-2-penteno foram combinados com o grupo alcoxisilano cloropropiltrimetoxisilano (CPTMS) e ancorado covalentemente aos suportes mesoporosos MCM-41 e SBA-15, coordenados pela intera??o com os grupos silan?is da matriz das s?licas e complexados com n?quel. Os complexos Ni-?-diimina/mesoporosos foram sintetizados para aplica??o em rea??es de oligomeriza??o do etileno e do propileno e para compara??o dos resultados entre o sistema homog?neo com o sistema heterog?neo. O suporte foi primeiramente sintetizado e calcinado. Ap?s foi realizado o ancoramento dos ligantes e posterior complexac?o do n?quel. Estes materiais foram caracterizados por v?rias t?cnicas, tais como: RMN de 1H, 13C e 29Si, DRX de baixo ?ngulo, Infra-vermelho (IR), an?lise termogravim?trica, an?lise de isotermas de adsor??o-dessor??o de N2, microscopia eletr?nica de transmiss?o (MET) e de varredura (MEV), an?lise elementar e espectroscopia de absor??o at?mica para confirmar o sucesso das s?nteses dos materiais. Ambos os complexos homog?neos e os heterogeneizados s?o ativos e seletivos para as rea??es de oligomeriza??o do etileno e do propileno. Os materiais heterogeneizados foram menos ativos que os complexos an?logos homog?neos nas rea??es de oligomeriza??o do etileno, por?m, foram mais seletivos tanto para fra??es C4 quanto para ?-C4. Nas rea??es com o propileno os complexos homog?neos promoveram ? rea??o de dimeriza??o e os complexos heterogeneizados ? rea??o de alquila??o do tolueno com o propileno. / The ?-diimine ligands 2-(phenyl)amine-4-(phenyl)imine-2-pentene and 2-(2,6-
dimethylphenyl)amine-4-(2,6-dimethylphenyl)imine-2-pentene were combined with the
alkoxysilane group chloropropyltrimethoxysilane (CPTMS) and covalently anchored to
a mesoporous MCM-41, Al-MCM-41 and SBA-15 support, ordered by interaction with
the silanols of the silica matrix and complexed with nickel. The complexes were
synthesized for application in ethylene and propylene oligomerization and for
comparing results between homogeneous and heterogeneous systems. The support is
first synthesized, calcined, anchored to the ligand, and then subsequent complexation of
nickel is realized. These materials were characterized by several techniques such as 1H,
13C and 29Si NMR, small angle XRD, Infra-red, thermogravimetric analysis, nitrogen
adsorption-desorption isotherms, transmission and scanning electron microscopy,
elemental analysis, and flame atomic absorption spectroscopy, to confirm the success of
the synthesis. Both homogeneous and heterogeneous complexes are active and selective
for the reactions of ethylene and propylene oligomerization. The heterogenized
materials were less active than the homogeneous analogous complexes in the reactions
of oligomerization of ethylene, however, were more selective for both C4 fractions and
for ?-C4. In reactions with propylene, the homogeneous complexes promoted the
dimerization reaction and the heterogenized complexes the alkylation reaction of
toluene with propylene complex.Complexes were tested in recycle reactions proved to
be efficient for use in large scale.
| Identifer | oai:union.ndltd.org:IBICT/oai:repositorio.ufrn.br:123456789/20557 |
| Date | 31 July 2015 |
| Creators | Rossetto, En?derson |
| Contributors | 50942611004, http://lattes.cnpq.br/5249001430287414, Santos, Eduardo Nicolau dos, 10210721847, http://lattes.cnpq.br/9246600674685393, Vitor Sobrinho, Eledir, 64656969915, http://lattes.cnpq.br/8488499388852606, Souza, Michele Oberson de, 58048472015, http://lattes.cnpq.br/3536832030182279, Braga, Tiago Pinheiro, 00880643366, http://lattes.cnpq.br/9170391410490804, Gusm?o, K?tia Bernardo, Pergher, Sibele Berenice Castella |
| Publisher | Universidade Federal do Rio Grande do Norte, PROGRAMA DE P?S-GRADUA??O EM QU?MICA, UFRN, Brasil |
| Source Sets | IBICT Brazilian ETDs |
| Language | Portuguese |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, info:eu-repo/semantics/doctoralThesis |
| Source | reponame:Repositório Institucional da UFRN, instname:Universidade Federal do Rio Grande do Norte, instacron:UFRN |
| Rights | info:eu-repo/semantics/openAccess |
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