Hydrocarbon oxidation by homogeneous and heterogeneous non-heme iron (III) catalysts with H2O2

被引:34
作者
Bilis, G. [1 ]
Christoforidis, K. C. [2 ]
Deligiannakis, Y. [2 ]
Louloudi, M. [1 ]
机构
[1] Univ Ioannina, Dept Chem, GR-45110 Ioannina, Greece
[2] Univ Ioannina, Dept Environm & Nat Resources Management, Phys Chem Lab, Agrinion 30100, Greece
关键词
Non-heme iron; Biomimetic catalysis; Hydrocarbon oxidation; H2O2; Fe-OOH; Low spin Fe; ELECTRON-PARAMAGNETIC-RESONANCE; OLEFIN CIS-DIHYDROXYLATION; SPIN IRON(III) COMPLEXES; DIOXYGEN ACTIVATION; METHANE MONOOXYGENASE; ALKANE HYDROXYLATION; HYDROGEN-PEROXIDE; CHEMISTRY; ENZYMES; EPOXIDATION;
D O I
10.1016/j.cattod.2010.03.063
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Homogeneous (LFeIII) and heterogeneous (LFeIII SiO2) [L = 3-{2-[2-(3-hydroxy-1 3-diphenyl-allylideneamino)-ethylamino]-ethylimino}-1 3-diphenyl propen-1-ol] catalysts have been synthesized and evaluated catalytically In CH3CN both the homogeneous and heterogeneous catalysts were efficient in alkene oxidations Cyclohexane oxidation provides total yield of 12 1% and 73% with an alcohol/ketone (A/K) ratio of 1 75 and 1 60 by the LFeIII and the LFeIII SiO2 catalysts respectively UV-vis kinetic data suggest formation of LFeIII-OOH species EPR data show that in the presence of CH3CN low-spin Fe-III (S = 1/2) centers are formed which are responsible for the catalytic activity The heterogeneous LFe SiO2 catalyst tested up to 5 re-uses shows a total yield loss similar to 4% per use providing the same distribution of oxidation products (C) 2010 Elsevier B V All rights reserved
引用
收藏
页码:101 / 106
页数:6
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