Mono- and binuclear complexes of iron(II) and iron(III) with an N4O ligand: synthesis, structures and catalytic properties in alkane oxidation

Li F; Wang M; Ma CB; Gao AP; Chen HB; Sun LC

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Mono- and binuclear complexes of iron(II) and iron(III) with an N4O ligand: synthesis, structures and catalytic properties in alkane oxidation

机译：具有N4O配体的铁（II）和铁（III）的单核和双核配合物：烷烃氧化的合成，结构和催化性能

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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).

机译：三种单核铁配合物和一种双核铁配合物[Fe（tpoen）Cl]中心点0.5（Fe2OCl6）（1），[Fe（tpoen）Cl] PF6（2），Fe（tpoen）Cl-3（3）和[{Fe（tpoen）}（2）（mu-O）]（ClO4）（4）（4）（tpoen = N-（2-吡啶基甲氧基乙基）-N，N-双（2-吡啶基甲基）胺）合成非血红素铁氧化酶的功能模型。晶体学研究表明，Fe（II）中心为1，处于伪八面体环境中，具有五齿N4O配体和一个氯离子转移到氧原子上。 3的Fe（III）中心以面部构型与三元的三个氮原子和三个氯离子连接。每个Fe（III）中心4与四个氮原子和一个氧原子氧原子配位，且Fe-O-Fe角为172.0（3）埃。配合物2、3和4在总TN中（A / K比为1.9-2.4）以H2O2催化环己烷与H2O2的氧化。在相同条件下，它们还催化了乙苯氧化为苯甲醇，苯甲醇和乙苯，并具有良好的活性（30-47 TN）和低选择性（A / K 0.7），以及金刚烷的氧化具有中等的活性（15-18 TN）。和低区域选择性（3度/ 2度3.0-3.2）。用mCPBA作为氧化剂，对于环己烷和乙苯的氧化，2、3和4的催化活性增加了1.8至2.3倍，对于金刚烷的氧化，其催化活性增加了6.3至7.5倍。在金刚烷的氧化中观察到区域选择性的急剧增强（3度/ 2度18.5-30.3）。

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《Dalton transactions: An international journal of inorganic chemistry》 |2006年第20期|共8页
作者
Li F; Wang M; Ma CB; Gao AP; Chen HB; Sun LC;
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正文语种 eng
中图分类无机化学;
关键词
SPECTROSCOPIC CHARACTERIZATION; PENTADENTATE LIGAND; NITROGEN LIGANDS; NONHEME; HYDROXYLATION; MODELS; FE(II); H2O2; INTERMEDIATE; ACETONITRILE;

机译：光谱表征;戊二烯配体;氮配体;非血红素;羟基氧化;模型;FE（II）;H2O2;中间体;乙腈;

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1. Mono- and binuclear complexes of iron(II) and iron(III) with an N4O ligand: synthesis, structures and catalytic properties in alkane oxidation [J] . Li F, Wang M, Ma CB, Dalton transactions: An international journal of inorganic chemistry . 2006,第20期

机译：具有N4O配体的铁（II）和铁（III）的单核和双核配合物：烷烃氧化的合成，结构和催化性能
2. Iron(III) complexes as superoxide dismutase mimics: Synthesis, characterization, crystal structure, and superoxide dismutase (SOD) activity of iron(III) complexes containing pentaaza macrocyclic ligands [J] . Zhang D., Lennon PL., Weiss RH., Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics . 1998,第5期

机译：铁（III）配合物作为超氧化物歧化酶的模拟物：含有五氮杂大环配体的铁（III）配合物的合成，表征，晶体结构和超氧化物歧化酶（SOD）活性
3. Synthesis, structures and catalytic properties of iron(III) complexes with asymmetric N-capped tripodal NO3 ligands and a pentadentate N2O3 ligand [J] . Tong LH, Wong YL, Pascu SI, Dalton transactions: An international journal of inorganic chemistry . 2008,第35期

机译：具有不对称N封端的三脚NO3配体和五齿N2O3配体的铁（III）配合物的合成，结构和催化性能
4. MONO- AND BINUCLEAR IRON COMPLEXES IN ZEOLITES AND MESOPOROUS OXIDES AS BIOMIMETIC ALKANE OXIDATION CATALYSTS [C] . NATO advanced study institute on catalytic activation and functionalisation of light alkanes . 1998

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6. Mono- and Dinuclear Iron Complexes of Bis(1-methylimidazol-2-yl)ketone (bik): Structure Magnetic Properties and Catalytic Oxidation Studies [O] . Pieter C. A. Bruijnincx, Inge L. C. Buurmans, Yuxing Huang, -1

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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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