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首页> 外文期刊>Chemistry: A European journal >The Series of Rare Earth Complexes [Ln_2Cl_6(m-4,4'-bipy)(py)_6], Ln=Y, Pr, Nd, Sm-Yb: A Molecular Model System for Luminescence Properties in MOFs Based on LnCl_3 and 4,4'-Bipyridine
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The Series of Rare Earth Complexes [Ln_2Cl_6(m-4,4'-bipy)(py)_6], Ln=Y, Pr, Nd, Sm-Yb: A Molecular Model System for Luminescence Properties in MOFs Based on LnCl_3 and 4,4'-Bipyridine

机译：稀土配合物系列[Ln_2Cl_6（m-4,4'-bipy）（py）_6]，Ln = Y，Pr，Nd，Sm-Yb：基于LnCl_3和4的MOF发光特性的分子模型系统，4'-联吡啶

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摘要

A series of 12 dinuclear complexes [Ln_2Cl_6(m-4,4'-bipy)(py)_6], Ln= Y, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, (1–12, respectively) was synthesized by an anhydrous solvothermal reaction in pyridine. The complexes contain a 4,4'-bipyridine bridge and exhibit a coordination sphere closely related to luminescent lanthanide MOFs based on LnCl_3 and 4,4-bipyridine. The dinuclear complexes therefore function as a molecular model system to provide a better understanding of the luminescence mechanisms in the Ln-N-MOFs _∞~2[Ln_2Cl_6(4,4'-bipy)_3]·2(4,4'-bipy). Accordingly, the luminescence properties of the complexes with Ln=Y, Sm, Eu, Gd, Tb, Dy, (1, 4–8) were determined, showing an antenna effect through a ligand–metal energy transfer. The highest efficiency of luminescence is observed for the terbium-based compound 7 displaying a high quantum yield (QY of 86%). Excitation with UV light reveals typical emission colors of lanthanide-dependent intra 4f–4f-transition emissions in the visible range (Tb~(III): green, Eu~(III): red, Sm~(III): salmon red, Dy~(III): yellow). For the Gd~(III)- and YIII-containing compounds 6 and 1, blue emission based on triplet phosphorescence is observed. Furthermore, ligand-to-metal charge-transfer (LMCT) states, based on the interaction of Cl~- with Eu~(III), were observed for the Eu~(III) compound 5 including energy-transfer processes to the EuIII ion. Altogether, the model complexes give further insights into the luminescence of the related MOFs, for example, rationalization of Ln-independent quantum yields in the related MOFs.
机译：一系列12个双核配合物[Ln_2Cl_6（m-4,4'-bipy）（py）_6]，Ln = Y，Pr，Nd，Sm，Eu，Gd，Tb，Dy，Ho，Er，Tm，Yb， （分别为1–12）是通过吡啶中的无水溶剂热反应合成的。该配合物包含4,4'-联吡啶桥，并显示出与基于LnCl_3和4,4-联吡啶的发光镧系元素MOF密切相关的配位球。因此，双核配合物起分子模型系统的作用，以更好地了解Ln-N-MOFs_∞〜2 [Ln_2Cl_6（4,4'-bipy）_3]·2（4,4'- bipy）。因此，确定了Ln = Y，Sm，Eu，Gd，Tb，Dy（1、4-8）的配合物的发光性质，显示了通过配体-金属能量转移的天线效应。对于显示出高量子产率（QY为86％）的b基化合物7，观察到最高的发光效率。紫外光激发显示可见光范围内镧系元素依赖的4f-4f跃迁发射的典型发射颜色（Tb〜（III）：绿色，Eu〜（III）：红色，Sm〜（III）：鲑鱼红，Dy 〜（III）：黄色）。对于含Gd（III）和YIII的化合物6和1，观察到基于三重态磷光的蓝色发射。此外，基于Cl〜-与Eu〜（III）的相互作用，对Eu〜（III）化合物5观察到了配体到金属的电荷转移（LMCT）状态，包括向EuIII离子的能量转移过程。总而言之，模型复合物为相关MOF的发光提供了进一步的见解，例如，在相关MOF中合理化了Ln无关的量子产率。

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