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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Synthesis, structural studies, and redox chemistry of bimetallic [Mn(CO)(3)] and [Re(CO)(3)] complexes
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Synthesis, structural studies, and redox chemistry of bimetallic [Mn(CO)(3)] and [Re(CO)(3)] complexes

机译：双金属[Mn（CO）（3）]和[Re（CO）（3）]复合物的合成，结构研究和氧化还原化学

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摘要

Manganese ([Mn(CO)(3)]) and rhenium tricarbonyl ([Re(CO)(3)]) complexes represent a workhorse family of compounds with applications in a variety of fields. Here, the coordination, structural, and electrochemical properties of a family of mono- and bimetallic [Mn(CO)(3)] and [Re(CO)(3)] complexes are explored. In particular, a novel heterobimetallic complex featuring both [Mn(CO)(3)] and [Re(CO)(3)] units supported by 2,2 '-bipyrimidine (bpm) has been synthesized, structurally characterized, and compared to the analogous monomeric and homobimetallic complexes. To enable a comprehensive structural analysis for the series of complexes, we have carried out new single crystal X-ray diffraction studies of seven compounds: Re(CO)(3)Cl(bpm), anti-[{Re(CO3)Cl}(2)(bpm)], Mn(CO)(3)Br(bpz) (bpz = 2,2 '-bipyrazine), Mn(CO)(3)Br(bpm), syn- and anti-[{Mn(CO3)Br}(2)(bpm)], and syn-[Mn(CO3)Br(bpm)Re(CO)(3)Br]. Electrochemical studies reveal that the bimetallic complexes are reduced at much more positive potentials (Delta E >= 380 mV) compared to their monometallic analogues. This redox behavior is consistent with introduction of the second tricarbonyl unit which inductively withdraws electron density from the bridging, redox-active bpm ligand, resulting in more positive reduction potentials. [Re(CO3)Cl](2)(bpm) was reduced with cobaltocene; the electron paramagnetic resonance spectrum of the product exhibits an isotropic signal (near g = 2) characteristic of a ligand-centered bpm radical. Our findings highlight the facile synthesis as well as the structural characteristics and unique electrochemical behavior of this family of complexes.
机译：锰（[Mn（CO）（3）]）和三羰基铼（[Re（CO）（3）]）配合物代表了一个主要的化合物家族，在许多领域都有应用。本文探讨了一系列单金属和双金属[Mn（CO）（3）]和[Re（CO）（3）]配合物的配位、结构和电化学性质。特别是，合成了一种新型的杂双金属配合物，其特征是[Mn（CO）（3）]和[Re（CO）（3）]单元均由2,2'-联吡啶（bpm）支撑，并对其结构进行了表征，并与类似的单体和均双金属配合物进行了比较。为了对这一系列配合物进行全面的结构分析，我们对七种化合物进行了新的单晶X射线衍射研究：Re（CO）（3）Cl（bpm）、anti-[{Re（CO3）Cl}（2）（bpm）]、Mn（CO）（3）Br（bpz）（bpz=2,2'-联吡嗪）、Mn（CO）（3）Br（bpm）、syn-和anti-[Mn（CO3）Br}（2）（bpm）]、syn-[Mn（CO3）Br（bpm）Re（CO）（3）Br（bpm）和syn-[Mn（CO 3）Br（bpm）]。电化学研究表明，与单金属类似物相比，双金属配合物在更高的正电位（δE>=380 mV）下被还原。这种氧化还原行为与引入第二个三羰基单元相一致，该单元感应性地从桥接、氧化还原活性bpm配体中提取电子密度，从而产生更多正还原电位。[Re（CO3）Cl]（2）（bpm）被钴酞菁还原；产物的电子顺磁共振光谱显示出以配体为中心的bpm自由基的各向同性信号（接近g=2）。我们的研究结果强调了这类配合物的简单合成、结构特征和独特的电化学行为。

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