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首页> 外文期刊>Chemistry: A European journal >Wire-Type Ruthenium(II) Complexes with Terpyridine-Containing [2]Rotaxanes as Ligands:Synthesis,Characterization,and Photophysical Properties
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Wire-Type Ruthenium(II) Complexes with Terpyridine-Containing [2]Rotaxanes as Ligands:Synthesis,Characterization,and Photophysical Properties

机译：含联吡啶的[2]轮烷作为配体的线型钌（II）配合物：合成，表征和光物理性质

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摘要

[2]Rotaxanes based on the 1,2-bis(pyridinium)ethanec[24]crown-8 ether motif were prepared that contain a terminal terpyridine group for coordination to a transition-metal ion.These rotaxane ligands were utilized in the preparation of a series of hetero-leptic [Ru(terpy)(terpy-rotaxane)]~(2+) complexes.The compounds were characterized by 1D and 2D ~1H NMR spec-troscopy,X-ray crystallography,and high-resolution electrospray ionization mass spectrometry.The effect of using a rotaxane as a ligand was probed by UV/Vis/NIR absorption and emission spectroscopy of the Ru~(II) complexes.In contrast with the parent [Ru(terpy)_2]~(2+) complex,at room temperature the examined complexes exhibit a lumines cence band in the near infrared region and a relatively long lived triplet metal-to-ligand charge-transfer (~3MLCT) excited state,owing to the presence of strong-electron-acceptor pyridinium substituents on one of the two terpy ligands.Visible-light excitation of the Ru-based chromophore in acetonitrile at room temperature causes an electron transfer to the cova-lently linked 4,4'-bipyridinium unit and the quenching of the MLCT luminescence.The ~3MLCT excited state,however,is not quenched at all in rigid matrix at 77 K.The rotaxane structure was found to affect the absorption and luminescence properties of the complexes.In particular,when a crown ether surrounds the cationic axle,the photoinduced electron-transfer process is slowed down by a factor from 2 to 3.Such features,together with the synthetic and structural advantages offered by [Ru(terpy)_2]~(2+)-type complexes compared to,for example,[Ru(bpy)_3]~(2+) -type compounds,render these rotax-ane-metal complexes promising candidates for the construction of photochemical molecular devices with a wire-type structure.
机译：制备了基于1,2-双（吡啶鎓）乙烷c [24] crown-8醚基序的轮烷，其包含一个末端联吡啶基团以与过渡金属离子配位。这些轮烷配体用于制备一系列杂配[Ru（terpy）（terpy-rotaxane）]〜（2+）配合物。通过1D和2D〜1H NMR光谱，X射线晶体学和高分辨率电喷雾电离对化合物进行表征通过Ru /（II）配合物的UV / Vis / NIR吸收和发射光谱研究轮状烷作为配体的效果。与母体[Ru（terpy）_2]〜（2+）形成对比络合物，在室温下，由于存在强电子受体吡啶鎓，所检测的络合物在近红外区显示出发光谱带，并且具有较长寿命的三重态金属-配体电荷转移（〜3MLCT）激发态两个三联配体之一上的取代基。在乙炔中Ru基发色团的可见光激发室温下的三氯甲烷会导致电子转移到与羰基连接的4,4'-联吡啶单元上，并导致MLCT发光猝灭。然而〜3MLCT的激发态在77 K的刚性基质中根本没有猝灭。发现轮烷结构会影响配合物的吸收和发光性能。特别是当冠醚围绕阳离子轴时，光致电子转移过程的速度降低了2到3倍。 [Ru（terpy）_2]〜（2+）型配合物与[Ru（bpy）_3]〜（2+）型化合物相比具有合成和结构优势，使这些rotax-烷金属配合物有望成为具有线型结构的光化学分子器件的构建候选。

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