Synthesis and application of Fe-III, Ni-II and Mn-II complexes anchored to HMS as efficient catalysts for cycloalkane oxyfunctionalization
authors Machado, K; Tavares, PB; Mishra, GS
nationality International
journal JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
author keywords Supported catalyst; Cyclohexane; O-2 oxidation; Batch reactor; Radical mechanism
keywords MODIFIED SILICA-GEL; H BOND ACTIVATION; CYCLOHEXANE OXIDATION; MOLECULAR-OXYGEN; HYDROCARBON OXIDATION; PEROXIDATIVE OXIDATION; ZEOLITE-Y; MCM-41; COPPER(II); DIOXYGEN
abstract Methoxysilane Schiff-base pentacoordinate metal complexes, Le. Fe[Sal(PMeO-Si)DPTA], Ni[Sal(PMeO-Si)DPTA] and Mn[Sal(PMeO-Si)DPTA], were synthesized and single site covalently anchored into the uniform porous texture of HMS (2-10 nm size) via condensation process. The correspondent supported catalysts (4.a, 4.b and 4.c, respectively) were characterized by FT-IR, SEM/EDS, XRD, TG, EPR and AAS analysis. In the catalytic tests, they showed high efficiency in the selective oxidation of cyclohexane using molecular O-2 (overall conversion 40.7% with Cat. 4.a, 29.5% with Cat. 4.b and 26.2% with Cat. 4.c) under relatively mild condition in batch reactor. The Cat.4.a system (HMS/3.a) exhibits highest TONs ca. 4.2 x 10(3) with good selectivity ca. 70% (48% ketone selectivity). The reaction mechanism involves free radicals, as it was proved by the addition of PPh3. Finally, these supported catalysts could be reuse up to several catalytic cycles. (C) 2013 Elsevier B.V. All rights reserved.
publisher ELSEVIER SCIENCE BV
issn 1381-1169
year published 2014
volume 383
beginning page 159
ending page 166
digital object identifier (doi) 10.1016/j.molcata.2013.12.004
web of science category Chemistry, Physical
subject category Chemistry
unique article identifier WOS:000333002000023
  ciceco authors
  impact metrics
dimensions (citation analysis):
altmetrics (social interaction):



 


Sponsors

1suponsers_list_ciceco.jpg