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首页> 外文期刊>Chemistry: A European journal >A unique case of oxidative addition of interhalogens IX (X=Cl, Br) to organodiselone ligands: Nature of the chemical bonding in asymmetric I-Se-X polarised hypervalent systems
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A unique case of oxidative addition of interhalogens IX (X=Cl, Br) to organodiselone ligands: Nature of the chemical bonding in asymmetric I-Se-X polarised hypervalent systems

机译：卤素间化合物IX（X = Cl，Br）氧化加成到有机二硒酮配体的独特情况：不对称I-Se-X极化高价体系中化学键的性质

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摘要

The reactivity of the imidazoline-2-selone derivatives 1,1′- methylenebis(3-methyl-4-imidazoline-2-selone) (D1) and 1,2-ethylenebis(3-methyl- 4-imidazoline-2-selone) (D2) towards the interhalogens IBr and ICl has been investigated in the solid state with the aim of synthesising "T-shaped" hypervalent chalcogen compounds featuring the extremely rare linear asymmetric I-E-X moieties (E=S, Se; X=Br, Cl). X-ray diffraction analysis and FT-Raman measurements provided a clear indication of the presence in the compounds obtained of discrete molecular adducts containing I-Se-Br and I-Se-Cl hypervalent moieties following a unique oxidative addition of interhalogens IX (X=Cl, Br) to the organoselone ligands. In all asymmetric hypervalent systems isolated, a strong polarisation was observed, with longer bond lengths at the selenium atom involving the most electronegative halogen. A topological electron density analysis on model compounds based on the quantum theory of atoms-in-molecules (QTAIM) and electron localisation function (ELF) established the three-centre-four-electron (3c-4e) nature of the bonding in these very polarised selenium hypervalent systems and new criteria were suggested to define and ascertain the hypervalency of the selenium atoms in these and related halogen and interhalogen adducts.
机译：咪唑啉-2-硒酮衍生物1,1'-亚甲基双（3-甲基-4-咪唑啉-2-硒酮）（D1）和1,2-亚乙基双（3-甲基-4-咪唑啉-2-硒酮）的反应性）已研究了在固态下朝向卤代化合物IBr和ICl的（D2），目的是合成具有极为罕见的线性不对称IEX部分（E = S，Se; X = Br，Cl ）。 X射线衍射分析和FT拉曼测量提供了清楚的指示，表明在化合物中存在离散的含I-S​​e-Br和I-Se-Cl高价部分的分子加合物，经过独特的氧化间卤素IX添加后（X = Cl，Br）形成有机硅配体。在所有孤立的不对称高价系统中，观察到强烈的极化，硒原子中的负电性最大的键长更长。基于分子中的量子理论（QTAIM）和电子本地化功能（ELF）对模型化合物进行拓扑电子密度分析，确定了在这些原子中键的三中心四电子（3c-4e）性质提出了极化的硒高价体系和新的标准，以定义和确定这些及相关卤素和卤素间加合物中硒原子的高价。

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