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首页> 外文期刊>Chemistry: A European journal >Influence of the Protonic State of an Imidazole-Containing Ligand on the Electrochemical and Photophysical Properties of a Ruthenium(II)-Polypyridine-Type Complex
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Influence of the Protonic State of an Imidazole-Containing Ligand on the Electrochemical and Photophysical Properties of a Ruthenium(II)-Polypyridine-Type Complex

机译：含咪唑的配体的质子态对钌（II）-聚吡啶类配合物的电化学和光物理性质的影响

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摘要

The synthesis and characterisation of [Ru(bpy)_2(PhenImHPh)]~(2+) where PhenImHPh represents the 2-(3,5-di-tert-butylphenyl)imidazo[4,5-f]-[1,10]phenanthroline ligand are described. The compounds issued from the three different protonic states of the imidazole ring [Ru(bpy)_2-(PhenImPh)]~+ (I), [Ru(bpy)_2(Phen-ImHPh)]~(2+) (II) and [Ru(bpy)_2(Phen-ImH_2Ph)]~(3+) (III) were isolated and spectroscopically characterised. The X-ray structures of [Ru(bpy)_2(Phen-ImPh)](PF_6) centre dot H2O centre dot 6MeOH, [Ru(bpy)_2-(PhenImHPh)] (NO3)2 centre dot H2O centre dot 3 MeOH and [Ru(bpy)_2(PhenImH_2Ph)] (PF_6)_3 centre dot 5H2O are reported. Electrochemical data obtained on these complexes indicate almost no potential shift for the Ru~(III/II) redox couple. Therefore a Cou-lombic effect between the imidazole ring and the metal centre can be ruled out. The monooxidised forms of I and II have been characterised by EPR spectroscopy and are reminiscent of the presence of a radical species. The emission properties of the parent com-pound [Ru(bpy)_2(PhenImHPh)]~(2+) were studied as a function of pH and both the lifetimes and intensities decreased upon deprotonation. Photophysical properties, investigated in the absence and presence of an electron acceptor (methylviologen), were distinctly different for the three compounds. Transient absorption features indicate that unique excited states are involved. Theoretical data obtained from DFT calculations in water on the three protonic forms are presented and discussed in the light of the experimental results.
机译：[Ru（bpy）_2（PhenImHPh）]〜（2+）的合成与表征，其中PhenImHPh代表2-（3,5-二叔丁基苯基）咪唑[4,5-f]-[1,10描述了菲咯啉配体。由咪唑环[Ru（bpy）_2-（PhenImPh）]〜+（I），[Ru（bpy）_2（Phen-ImHPh）]〜（2+）的三个不同质子态发出的化合物并分离[Ru（bpy）_2（Phen-ImH_2Ph）]〜（3+）（III）并进行光谱表征。 [Ru（bpy）_2（Phen-ImPh）]（PF_6）中心点H2O中心点6MeOH，[Ru（bpy）_2-（PhenImHPh）]（NO3）2中心点H2O中心点3 MeOH的X射线结构和[Ru（bpy）_2（PhenImH_2Ph）]（PF_6）_3中心点5H2O被报告。在这些络合物上获得的电化学数据表明，Ru〜（III / II）氧化还原对几乎没有电位移动。因此，可以排除咪唑环与金属中心之间的库仑效应。 I和II的单氧化形式已通过EPR光谱进行了表征，让人联想到自由基的存在。研究了母体化合物[Ru（bpy）_2（PhenImHPh）]〜（2+）的发射性质与pH的关系，去质子化后寿命和强度均降低。对于三种化合物，在不存在和存在电子受体（甲基紫精）的情况下研究的光物理性质明显不同。瞬态吸收特征表明涉及独特的激发态。根据实验结果，介绍和讨论了在水中以三种质子形式通过DFT计算获得的理论数据。

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