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首页> 外文期刊>Chemistry: A European journal >Synthesis, Coordination Chemistry and Bonding of Strong N-Donor Ligands Incorporating the 1H-Pyridin-(2E)-Ylidene (PYE) Motif
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Synthesis, Coordination Chemistry and Bonding of Strong N-Donor Ligands Incorporating the 1H-Pyridin-(2E)-Ylidene (PYE) Motif

机译：含1H-吡啶-（2E）-亚烷基（PYE）母体的强N配体配体的合成，配位化学和键合

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摘要

A range of N-donor ligands based on the 1H-pyridin-(2E)-ylidene (PYE) motif have been prepared, including achiral and chiral examples. The ligands incorporate one to three PYE groups that coordinate to a metal through the exocyclic nitrogen atom of each PYE moiety, and the resulting metal complexes have been characterised by methods including single-crystal X-ray diffraction and NMR spectroscopy to examine metal–ligand bonding and ligand dynamics. Upon coordination of a PYE ligand to a proton or metal-complex fragment, the solidstate structures, NMR spectroscopy and DFT studies indicate that charge redistribution occurs within the PYE heterocyclic ring to give a contribution from a pyridinium–amido-type resonance structure. Additional IR spectroscopy and computational studies suggest that PYE ligands are strong donor ligands. NMR spectroscopy shows that for metal complexes there is restricted motion about the exocyclic CN bond, which projects the heterocyclic N-substituent in the vicinity of the metal atom causing restricted motion in chelating-ligand derivatives. Solid-state structures and DFT calculations also show significant steric congestion and secondary metal–ligand interactions between the metal and ligand CH bonds.
机译：已经制备了基于1H-吡啶-（2E）-亚烷基（PYE）基序的一系列N-供体配体，包括非手性和手性实例。配体结合了一个到三个PYE基团，这些PYE基团通过每个PYE部分的环外氮原子与金属配位，并且所得的金属络合物已通过包括单晶X射线衍射和NMR光谱法的方法进行了表征，以检查金属-配体的键合和配体动力学。在将PYE配体与质子或金属络合物片段配位后，固态结构，NMR光谱学和DFT研究表明，电荷在PYE杂环内发生了重新分布，从而产生了吡啶鎓-酰胺基型共振结构。额外的红外光谱和计算研究表明，PYE配体是强供体配体。 NMR光谱显示，对于金属络合物，环外CN键的运动受限，该键将杂环N-取代基投射到金属原子附近，从而导致螯合配体衍生物的运动受限制。固态结构和DFT计算也显示出明显的空间拥堵以及金属与配体CH键之间的次生金属-配体相互作用。

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