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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Molecular Design of pH-Sensitive Ru(II)-Polypyridyl Luminophores
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Molecular Design of pH-Sensitive Ru(II)-Polypyridyl Luminophores

机译：pH敏感ru（II）-polypyridyl发光体的分子设计

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摘要

Three new [Ru(bpy)(2)X](+) complex ions, where bpy represents bipyridyl ligand and X denotes pyridyl diazolate or pyrazinyl diazolate coordination site, have been computationally designed and synthesized as pH-sensitive molecules. The choice of pyridyl and pyrazinyl moieties allows for the nitrogen content to vary, whereas the influence of the protonation site is quantified by using 1,2-diazolate and 1,3-diazolate derivatives. The absorption and emission properties of the deprotonated and protonated complex ions were characterized by UV-vis and photoluminescence spectroscopy as well as by time-dependent density functional theory. Protonation causes (1) a strong blue shift in the lowest energy (MLCT)-M-3 -> S-0 emission wavelengths, (2) a substantial increase in the emission intensity, and (3) a change in the character of the corresponding (MLCT)-M-3 emitting states. The blue shift in the emission wavelength becomes less pronounced when the nitrogen content in the X-ligand increases and when going from 1,2- to 1,3-diazolate derivatives. The contrast in the emission intensity of the protonated/deprotonated forms is the highest for the complex ion, containing a 2-pyridyl derivative of the 1,2-diazolate. The complex ions are suggested as potential pH-responsive materials based on change in the color and intensity of the emitted radiation. The broad impact of the research demonstrates that the modification of the nitrogen content and position within the protonable ligands is an effective approach for modulation of the pH-optosensing properties of Ru-polypyridyl complexes.
机译：三种新的[Ru（BPY）（2）x]（+）复合离子，其中Bpy代表双吡啶基配体和X表示吡啶基二元酸盐或吡嗪基二元酸盐配位部位，已经计算设计和合成为pH敏感分子。吡啶基和吡嗪基部分的选择允许氮含量变化，而质子化位点的影响通过使用1,2-二氮化物和1,3-二元衍生物来定量。通过UV-Vis和光致发光光谱以及通过时间依赖性密度函数理论，表征了质子化和质子化的复合离子的吸收和排放性能。质子化导致（1）最低能量（MLCT）-M-3 - > S-0发射波长的强烈蓝色偏移，（2）发射强度的大幅增加，（3）变化的变化相应的（MLCT）-M-3发射状态。当X-配体中的氮含量增加并且从1,2-至1,3-二氮化衍生物的衍生物增加时，发射波长中的蓝色移位变得更加明显。质子化/质子化形式的发射强度的对比度是复合离子的最高，含有1,2-二元化物的2-吡啶基衍生物。基于发出辐射的颜色和强度的变化，建议复合离子作为潜在的pH响应材料。该研究的广泛影响表明，质子化配体内的氮含量和位置的改性是用于调节Ru-聚吡啶络合物的pH-光致溶剂性能的有效方法。

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