Single site anchored novel pentacoordinate Schiff-base Co-(II) complexes over SBA-15 for selective oxidation (O-2) of n-alkanes and kinetic study

• Tipo: Artigo em Revista Científica Internacional
• Data: 2014

Autores

Kelly Machado (Autor) Outra; Pedro B Tavares (Autor) Outra; Cristina Freire (Autor) FCUP; Gopal S Mishra (Autor) Outra

Revista

Título: Polyhedron

Vol. 69

Páginas: 119-126

ISSN: 0277-5387

Editora: Elsevier

Indexação

ISI Web of Knowledge - 4 Citações

Scopus - 4 Citações

Classificação Científica

FOS: Ciências exactas e naturais > Química

Outras Informações

ID Authenticus: P-008-JTD

DOI: 10.1016/j.poly.2013.11.025

Abstract (EN): Trimethoxysilane pentacoordinate Schiff-base Co-(II) complexes, i.e. Co[Cl-Sal(PMeO-Si)DPTA], (3.a) and Co[F-Sal(PMeO-Si)DPTA], (3.b) and Co[FCl-Sal(PMeO-Si)DPTA], (3.c) (DPTA = bis(aminopropyl)amine, Sal = salicylaldehyde) were synthesized and anchored into SBA-15 matrix to obtain novel supported hybrid catalysts. The catalysts were characterized by FT-IR, TEM, SEM, XRD, TG and BET analysis. These supported complex catalysts were tested in the catalytic oxidation of n-hexane and n-heptane with O-2 under relatively mild and solvent free conditions. A high TON of 3320 with 19.6% yield for n-hexane oxidation and a high TON of 3180 with 17.3% yield for n-heptane oxidation were obtained with 3.b anchored over SBA-15. The oxidation product regioselectivities were obtained as C-1(1):C-2(9.2):C-3(10.7) for n-hexane and C-1(1):C-2(9.0):C-3(9.7):C-4(2.7) for n-heptane. The reaction of kinetics follows a pseudo first-order reaction for both n-alkanes. Enhanced yields (30.6% for n-hexane oxidation and 23.8% for n-heptane oxidation) were obtained with the addition of PCA (pyrazinecarboxylic acid); the catalytic results of reactions made in the presence of radical traps suggested that the catalytic oxidation of n-hexane and n-heptane proceeded via free radicals. The catalyst recycles tests showed that it could be reused up to 7th catalytic cycles.

Idioma: Inglês

Tipo (Avaliação Docente): Científica

Nº de páginas: 8