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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Formation, reactivity and redox properties of carbon- and sulfur-bridged diiron complexes derived from dibenzothienyl Schiff bases: effect of N,N- and N,P-chelating moieties
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Formation, reactivity and redox properties of carbon- and sulfur-bridged diiron complexes derived from dibenzothienyl Schiff bases: effect of N,N- and N,P-chelating moieties

机译：衍生自二苯并噻吩基席夫碱的碳桥和硫桥联二铁配合物的形成，反应性和氧化还原特性：N，N和N，P螯合部分的作用

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摘要

Dibenzothienyl Schiff bases, DBT-NN and DBT-NP, were derived from condensation of 4-formyldibenzothiophene with N,N-dimethylethylenediamine and 2-(diphenylphosphino)ethylamine, respectively. A photochemical reaction of [Fe(CO)(5)] with DBT-NN produced diiron complexes, [Fe-2(mu-DBT-NN)(CO)(6)] (1) and [{Fe(mu-BPT-NN-kappa S-3,C,N)(CO)(2)} Fe(CO)(3)] (2). Complex 1 has pi coordination of a Schiff base C=N bond and an N,N-chelate, while 2 has an S,C,N-tridentate ligand having an uncoordinated dimethylamino group. The corresponding reaction with DBT-NP produced a diiron complex of an S,C,N,P-tetradentate ligand, [{Fe(mu-BPT-NP-kappa S-4,C,N,P)(CO)}Fe(CO)(3)] (3), which has an N,P-chelate, via the DBT-NP complex [Fe(DBT-NP-kappa P)(CO)(4)] (4). Reactions of 2 and 3 with one equivalent of PMe2Ph gave the monosubstituted complexes [{Fe(mu-BPT-NN-kappa S-3,C,N)(CO)(2)}Fe(CO)(2)(PMe2Ph)] (5) and [{Fe(mu-BPT-NP-kappa S-4,C,N,P)(CO)}Fe(CO)(2)(PMe2Ph)] (6), respectively. The corresponding reactions with an excess of PMe2Ph produced mononuclear complexes, trans-[Fe(BPT-NN-kappa S-3,C,N)(CO)(PMe2Ph)(2)] (7) and [Fe(BPT-NP-kappa S-4,C,N,P)(CO)(PMe2Ph)] (8), respectively. Complexes 1-3 and 5-8 were structurally characterized by X-ray crystallography. Complexes 2, 3, 5 and 6 have similar dinuclear structures with different carbonyl/phosphine substitution patterns. Cyclic voltammograms of 2, 3 and 5 showed two one-electron reduction processes, and more negative potentials were observed for 6. The shift of the redox potentials are rationalized by the electron-donating character of the phosphine ligands, which suggests that the reduction occurs at the asymmetrically bridged diiron core.
机译：二苯并噻吩基席夫碱DBT-NN和DBT-NP分别来自4-甲酰基二苯并噻吩与N，N-二甲基乙二胺和2-（二苯基膦基）乙胺的缩合反应。 [Fe（CO）（5）]与DBT-NN生成的二铁配合物[Fe-2（mu-DBT-NN）（CO）（6）]（1）和[{Fe（mu-BPT） -NN-κS-3，C，N）（CO）（2）} Fe（CO）（3）]（2）。配合物1具有席夫碱C ＝ N键和N，N-螯合物的π配位，而配合物2具有具有未配位的二甲基氨基的S，C，N-三齿配体。与DBT-NP的相应反应产生S，C，N，P-四齿配体[{Fe（mu-BPT-NP-k S-4，C，N，P）（CO）} Fe的二铁配合物（CO）（3）]（3），它通过DBT-NP络合物[Fe（DBT-NP-κP）（CO）（4）]（4）具有N，P螯合物。 2和3与一当量的PMe2Ph反应得到单取代的配合物[{Fe（mu-BPT-NN-kappa S-3，C，N）（CO）（2）} Fe（CO）（2）（PMe2Ph） ]（5）和[{Fe（mu-BPT-NP-k S-4，C，N，P）（CO）} Fe（CO）（2）（PMe2Ph）]（6）。与过量PMe2Ph的相应反应产生了单核络合物，反式[Fe（BPT-NN-kappa S-3，C，N）（CO）（PMe2Ph）（2）]（7）和[Fe（BPT-NP -k S-4，C，N，P）（CO）（PMe2Ph）]（8）。配合物1-3和5-8通过X射线晶体学表征。配合物2、3、5和6具有相似的双核结构，具有不同的羰基/膦取代模式。 2、3和5的循环伏安图显示了两个单电子还原过程，并且在6处观察到更多的负电势。氧化还原电势的移动通过膦配体的供电子特性而合理化，这表明发生了还原在不对称桥接的狄龙铁心处。

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