Oxomolybdenum monodithiolene complexes linked with sulfur bridged iron: Antiferromagnetically coupled Fe(iii)Mo(v) systems

Moula G.; Bose M.; Maiti B.K.; Sarkar S.

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Oxomolybdenum monodithiolene complexes linked with sulfur bridged iron: Antiferromagnetically coupled Fe(iii)Mo(v) systems

机译：与硫桥铁连接的氧钼单二硫代苯配合物：反铁磁耦合的Fe（iii）Mo（v）系统

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Mo-Fe heterometallic complexes with Fe(X) _2 (X = Cl, SPh) moiety attached to monodithiolene oxomolybdenum via sulfur bridge, viz., [Ph _4P] _2[Cl _2FeS _2MoOS _2(DMED)] (2) (DMED, dimethylethylenedicarboxylate), [Ph _4P] _2[Cl _2FeS _2MoO(tdt)] (3) (tdt, toluenedithiolate) and [Ph _4P] _2[(SPh) _2FeS _2MoO(tdt)] (4) are reported. Mossbauer spectroscopy, magnetism, EPR, electrochemistry and electronic structure based on DFT and TD-DFT calculation show the transfer of electron from iron to molybdenum centre resulting antiferromagnetically coupled Fe(iii)Mo(v) unit from the starting Fe(ii) and Mo(vi) compounds. A net spin of S = 2 ground state arising from antiferromagnetically coupled Fe(iii) and Mo(v) shows a rare X-band EPR in normal mode at g ～ 12 in the solid state. In addition, Mossbauer studies show that electron drifting is more pronounced upon substitution of the chloride ligand by thiophenolate. The changes in dithiolene periphery electronically affect the charge distribution between Mo-Fe in {OMo(μS) _2Fe} core. DFT calculations indicate that the increasing stability of dative Fe → Mo hetero metal-metal bond in these complexes from 3 to 2 to 4 is related to the extent of electron transfer from the iron to molybdenum centre.

机译：具有Fe（X）_2（X = Cl，SPh）部分的Mo-Fe杂金属配合物，通过硫桥，即[Ph _4P] _2 [Cl _2FeS _2MoOS _2（DMED）]（2）（DMED，报告了[Ph _4P] _2 [Cl _2FeS _2MoO（tdt）]（3）（tdt，甲苯二硫醇盐）和[Ph _4P] _2 [（（SPh）_2FeS _2MoO（tdt）]（4）。基于DFT和TD-DFT计算的Mossbauer光谱学，磁性，EPR，电化学和电子结构显示电子从铁到钼中心的转移从起始Fe（ii）和Mo反铁磁耦合Fe（iii）Mo（v）单元（vi）化合物。反铁磁耦合的Fe（iii）和Mo（v）产生的S = 2基态净自旋表明，在固态下g〜12时，在正常模式下稀有X波段EPR。此外，Mossbauer的研究表明，在氯代配体被硫代酚酸酯取代后，电子漂移更为明显。在{OMo（μS）_2Fe}磁芯中，二硫辛烯外围的变化会电子地影响Mo-Fe之间的电荷分布。 DFT计算表明，在这些配合物中，Fe→Mo杂原子-金属键的稳定度从3增加到2至4与电子从铁到钼中心的转移程度有关。

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《Dalton transactions: An international journal of inorganic chemistry》 |2012年第41期|共10页
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Moula G.; Bose M.; Maiti B.K.; Sarkar S.;
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Oxomolybdenum monodithiolene complexes linked with sulfur bridged iron: Antiferromagnetically coupled Fe(iii)Mo(v) systems

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