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Mono- and binuclear...
Mono- and binuclear complexes of iron(II) and iron(III) with an N4O ligand : synthesis, structures and catalytic properties in alkane oxidation
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Li, F. (författare)
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Wang, M. (författare)
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Ma, C. B. (författare)
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Gao, A. P. (författare)
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Chen, H. B. (författare)
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Sun, Licheng C. (författare)
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- Royal Society of Chemistry (RSC), 2006
- 2006
- Engelska.
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Ingår i: Dalton Transactions. - : Royal Society of Chemistry (RSC). - 1477-9226 .- 1477-9234. ; :20, s. 2427-2434
- Relaterad länk:
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Three mononuclear iron complexes and one binuclear iron complex, [Fe(tpoen)Cl]center dot 0.5(Fe2OCl6) (1), [Fe(tpoen)Cl]PF6 (2), Fe(tpoen)Cl-3 (3) and [{Fe(tpoen)}(2)(mu-O)](ClO4)(4) (4) (tpoen = N-(2-pyridylmethoxyethyl)-N,N-bis(2-pyridylmethyl)amine), were synthesized as functional models of non-heme iron oxygenases. Crystallographic studies revealed that the Fe(II) center of 1 is in a pseudooctahedral environment with a pentadentate N4O ligand and a chloride ion trans to the oxygen atom. The Fe(III) center of 3 is ligated by three nitrogen atoms of tpoen and three chloride ions in a facial configuration. Each Fe(III) center of 4 is coordinated with four nitrogen atoms and an oxygen atom of tpoen with the Fe-O-Fe angle of 172.0(3) angstrom. Complexes 2, 3 and 4 catalysed the oxidation of cyclohexane with H2O2 in the total TNs of 24 - 36 with A/K ratios of 1.9-2.4. Under the same conditions they also catalysed both the oxidation of ethylbenzene to benzylic alcohol and acetobenzene with good activity (30-47 TN) and low selectivity (A/K 0.7), and the oxidation of adamantane with moderate activity (15-18 TN) and low regioselectivity (3 degrees/2 degrees 3.0-3.2). With mCPBA as oxidant the catalytic activities of 2, 3 and 4 increased 1.8 to 2.3-fold for the oxidation of cyclohexane and ethylbenzene and 6.3 to 7.5-fold for the oxidation of adamantane. Drastic enhancement of the regioselectivity was observed in the oxidation of adamantane (3 degrees/2 degrees 18.5-30.3).
Nyckelord
- spectroscopic characterization
- pentadentate ligand
- nitrogen ligands
- nonheme
- hydroxylation
- models
- fe(ii)
- h2o2
- intermediate
- acetonitrile
Publikations- och innehållstyp
- ref (ämneskategori)
- art (ämneskategori)
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