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Deciphering the photobehaviour of ensemble and single crystals of Zr-based ITQ MOF composites
Journal of Photochemistry and Photobiology A: Chemistry ( IF 4.3 ) Pub Date : 2020-09-06 , DOI: 10.1016/j.jphotochem.2020.112887
Elena Caballero-Mancebo , José María Moreno , Avelino Corma , Urbano Díaz , Boiko Cohen , Abderrazzak Douhal

Understanding the interactions that govern the photophysical behaviour of Metal-organic frameworks (MOFs) and their composites is paramount for their photochemical and photonic applications. In this work, we report on the photobehaviour of Nile Red (NR) adsorbed on the surface of 2D Zr-ITQ-HB ([email protected]) MOF using ultrafast (fs-ns) and single-molecule fluorescence techniques. The results show the occurrence of energy transfer processes happening in 0.34 ns between neighbouring NR molecules, intramolecular charge transfer reaction (∼0.6 ps) and a vibrational cooling (10 ps) of the adsorbed dye. Time-resolved single-composite fluorescence microscopy experiments on different NR-loaded composites allowed to resolve the emission from adsorbed aggregates (0.9 ns) and from the charge separated state (2.5 ns) of excited NR. The different photobehaviour of NR adsorbed on ZrO2 nanoparticles indicates the relevance of the Zr-ITQ-HB MOFs surface to the observed photoinduced reactions in the composites. We discuss how the nature of both, the organic linkers and metal clusters in this kind of MOFs, affects the photodynamics of the composites. These results may help in designing MOFs "on demand" for their application in photons-based science and technology, like photocatalysis and lighting.



中文翻译:

锆基ITQ MOF复合材料的整体和单晶的光学行为

了解控制金属有机骨架(MOF)及其复合物的光物理行为的相互作用对于其光化学和光子应用至关重要。在这项工作中,我们报告了使用超快(fs-ns)和单分子荧光技术吸附在2D Zr-ITQ-HB([受电子邮件保护])MOF表面的尼罗红(NR)的光行为。结果表明,相邻的NR分子之间在0.34 ns内发生了能量转移过程,分子内的电荷转移反应(约0.6 ps)和吸附染料的振动冷却(10 ps)发生了。在不同的NR负载的复合材料上进行时间分辨的单复合荧光显微镜实验,可以解析吸附的聚集体(0.9 ns)和激发的NR的电荷分离状态(2.5 ns)的发射。2个纳米粒子表明Zr-ITQ-HB MOF表面与复合物中观察到的光诱导反应的相关性。我们讨论了这种MOF中有机连接基和金属簇的性质如何影响复合材料的光动力学。这些结果可能有助于设计“按需” MOF,以将其应用于基于光子的科学技术中,例如光催化和照明。

更新日期:2020-09-20
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