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Anthracene-Based Lanthanide Metal-Organic Frameworks: Synthesis, Structure, Photoluminescence, and Radioluminescence Properties

机译:基于蒽的镧系金属 - 有机框架:合成,结构,光致发光和放射发光性能

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摘要

Four anthracene-based lanthanide metal-organic framework structures (MOFs) were synthesized from the combination of the lanthanide ions, Eu3+, Tb3+, Er3+, and Tm3+, with 9,10-anthracenedicarboxylic acid (H2ADC) in dimethylformamide (DMF) under hydrothermal conditions. The 3-D networks crystalize in the triclinic system with P-1 space group with the following compositions: (i) {{[Ln2(ADC)3(DMF)4·DMF]}n, Ln = Eu (1) and Tb (2)} and (ii) {{[Ln2(ADC)3(DMF)2(OH2)2·2DMF·H2O]}n, Ln = Er (3) and Tm (4)}. The metal centers exist in various coordination environments; nine coordinate in (i), while seven and eight coordinate in (ii). The deprotonated ligand, ADC, assumes multiple coordination modes, with its carboxylate functional groups severely twisted away from the plane of the anthracene moiety. The structures show ligand-based photoluminescence, which appears to be significantly quenched when compared with that of the parent H2ADC solid powder. Structure 2 is the least quenched and showed an average photoluminescence lifetime from bi-exponential decay of 0.3 ns. On exposure to ionizing radiation, the structures show radioluminescence spectral features that are consistent with the isolation of the ligand units in its 3-D network. The spectral features vary among the 3-D networks and appear to suggest that the latter undergo significant changes in their molecular and/or electronic structure in the presence of the ionizing radiation.
机译:从镧系元素,Eu3 +,Tb3 +,ER3 +和TM3 +的组合合成了四种基于蒽基的镧系元素 - 有机骨架结构(MOF),在水热条件下在二甲基甲酰胺(DMF)中具有9,10-蒽羧酸(H2ADC)的组合。 3-D网络在具有以下组合物的P-1空间组的三级网络中结晶:(i){{[Ln2(ADC)3(DMF)4·DMF]} N,LN = EU(1)和TB (2)}和(II){{[LN2(ADC)3(DMF)2(OH2)2·2DMF·H2O] N,LN = ER(3)和TM(4)}。金属中心存在于各种配位环境中; (i)九个坐标,而第七和八个坐标(ii)。去质子化配体ADC假设多种配位模式,其羧酸酯官能团严重扭转远离蒽部分的平面。该结构表明了与亲本H2ADC固体粉末相比显着淬火的配体基光致发光。结构2是最不淬火的,并且显示来自0.3ns的双指数衰减的平均光致发光寿命。在暴露于电离辐射时,结构示出了与其3-D网络中的配体单元隔离一致的放射致发光光谱特征。光谱特征在3-D网络中变化,并且似乎表明后者在电离辐射存在下在其分子和/或电子结构中经历显着变化。

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