Thermally induced stoichiometric and catalytic O-atom transfer by a non-heme iron(III)-nitro complex:: First example of reversible {Fe-NO}7⇆FeIII-NO2 transformation in the presence of dioxygen
被引:42
作者:
Patra, AK
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机构:Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
Patra, AK
Afshar, RK
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机构:Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
Afshar, RK
Rowland, JM
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机构:Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
Rowland, JM
Olmstead, MM
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机构:Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
Olmstead, MM
Mascharak, PK
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机构:
Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USAUniv Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
Mascharak, PK
[1
]
机构:
[1] Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
[2] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA
heterogeneous catalysis;
iron;
N ligands;
nitrogen oxides;
phosphanes;
D O I:
10.1002/anie.200352070
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
The non-heme iron(III) complex [(PaPy3)Fe(NO 2)](ClO4) (1) transfers oxygen in the temperature range 45-65 °C to PPh3 to afford OPPh3 in MeCN. The product, [(PaPy3)Fe(NO)](ClO4), a {Fe-NO}7 species, reverts rapidly back to 1 in the presence of dioxygen, thus making the system catalytic (see scheme). Formation of an oxo-bridged species terminates the oxo-transfer process (PaPy3H = N-[N,N-bis(2-pyridylmethyl)aminoethyl]-2-pyridinecarboxamide).