[FeFe]-hydrogenase H-cluster mimics mediated by mixed (S, Se) and (S, Te) bridging moieties: Insight into molecular structures and electrochemical characteristics

IF 1.1 4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Heteroatom Chemistry Pub Date : 2018-10-30 DOI:10.1002/hc.21446

Hassan Abul-Futouh, Mohammad El-khateeb, Helmar Görls, Wolfgang Weigand

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引用次数: 8

Abstract

Two synthetic models of the active site of [FeFe]-hydrogenase containing mixed (S, Se) and (S, Te) bridges have been synthesized and characterized. These complexes [Fe₂(CO)₆{μ-S(CH₂)₄E-μ)}] (E = Se (1), Te (2)) are obtained in moderate yields from the reaction of Fe₃(CO)₁₂ with 1,2-thiaselenane or 1,2-thiatellurane. They have been characterized by spectroscopic techniques (IR, ¹H-, ¹³C{¹H}-, ⁷⁷Se{¹H}-, ¹²⁵Te{¹H}-NMR, and MS) and elemental analysis. The structures of [Fe₂(CO)₆{μ-S(CH₂)₄Se-μ)}] and [Fe₂(CO)₆{μ-S(CH₂)₄Te-μ)}] are determined by X-ray structure determination and show the expected butterfly geometry. Moreover, the influence of the mixed chalcogen atoms on the redox properties and the catalytic behavior of 1 and 2 are studied using cyclic voltammetry.

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混合（S，Se）和（S，Te）桥接部分介导的[FeFe]-氢化酶H-簇模拟物：对分子结构和电化学特性的洞察

合成并表征了两种含(S, Se)和(S, Te)混合桥的[FeFe]-氢化酶活性位点的合成模型。这些配合物[Fe2(CO)6{μ-S(CH2)4E-μ)}] (E = Se (1)， Te(2))由Fe3(CO)12与1,2-硫乙烯或1,2-硫乙烷反应得到，产率中等。它们已通过光谱技术(IR, 1H-， 13C{1H}-， 77Se{1H}-， 125Te{1H}- nmr和MS)和元素分析进行了表征。用x射线结构测定法测定了[Fe2(CO)6{μ-S(CH2)4Se-μ)}]和[Fe2(CO)6{μ-S(CH2)4Te-μ)}]的结构，显示出预期的蝴蝶形状。此外，还利用循环伏安法研究了混合氯原子对1和2的氧化还原性能和催化行为的影响。

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来源期刊

Heteroatom Chemistry 化学-化学综合

CiteScore

1.20

自引率

0.00%

发文量

审稿时长

6 months

期刊介绍： Heteroatom Chemistry brings together a broad, interdisciplinary group of chemists who work with compounds containing main-group elements of groups 13 through 17 of the Periodic Table, and certain other related elements. The fundamental reactivity under investigation should, in all cases, be concentrated about the heteroatoms. It does not matter whether the compounds being studied are acyclic or cyclic; saturated or unsaturated; monomeric, polymeric or solid state in nature; inorganic, organic, or naturally occurring, so long as the heteroatom is playing an essential role. Computational, experimental, and combined studies are equally welcome. Subject areas include (but are by no means limited to): -Reactivity about heteroatoms for accessing new products or synthetic pathways -Unusual valency main-group element compounds and their properties -Highly strained (e.g. bridged) main-group element compounds and their properties -Photochemical or thermal cleavage of heteroatom bonds and the resulting reactivity -Uncommon and structurally interesting heteroatom-containing species (including those containing multiple bonds and catenation) -Stereochemistry of compounds due to the presence of heteroatoms -Neighboring group effects of heteroatoms on the properties of compounds -Main-group element compounds as analogues of transition metal compounds -Variations and new results from established and named reactions (including Wittig, Kabachnik–Fields, Pudovik, Arbuzov, Hirao, and Mitsunobu) -Catalysis and green syntheses enabled by heteroatoms and their chemistry -Applications of compounds where the heteroatom plays a critical role. In addition to original research articles on heteroatom chemistry, the journal welcomes focused review articles that examine the state of the art, identify emerging trends, and suggest future directions for developing fields.