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Solvothermal Synthesis of High-Performance d10-MOFs with Hydrogel Membranes @ “Turn-On” Monitoring of Formaldehyde in Solution and Vapor Phase

机译:用水凝胶膜的高性能D10-MOF合成甲醛溶液和气相中甲醛的高性能D10-MOF

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Herein, two luminescent porous networks (CMERI-1 & CMERI-2) have been reported for the efficient detection of formaldehyde (FA) from aqueous medium. Judicious solvent screening using a high-throughput solvothermal procedure leads to two completely different metal–organic framework (MOFs) with different architectures. It is perceived that the framework CMERI-1 shows better sensitivity with a very short response time (1 min) in the realm of FA detection due to the facile imine (?N═CH?) formation, which is restricted in the case of CMERI-2. The fluorescence “turn-on” behavior is ascribed due to the inhibition of photoinduced electron transfer (PET) (from amine subunit to secondary building unit) process. The detection limits of CMERI-1 & CMERI-2 toward FA in aqueous medium were found to be 0.62 μM (0.019 ppm) and 1.39 μM (0.041 ppm), respectively, that lie far below the intracellular concentration of formaldehyde (100–400 μM). In addition, MOF-based hydrogel membrane was fabricated, which shows vapor-phase detection of FA, which is hitherto unexplored in this realm. Moreover, the response mechanisms of MOFs are supported by density functional theory (DFT) and Fukui indices analysis. The high stability of the porous frameworks along with its interesting sensing features such as fast recognition phenomenon, appreciable detection limit, etc. instigated us to explore its real-world applicability in various food sample and water analyses. In view of the modular design principle of our polymeric probe, the proposed approach could open a new horizon to construct powerful sensing materials for the ultrafast detection of other industrial pollutants in the domain of supramolecular and analytical chemistry.
机译:本文报道了两种发光多孔网络(CMERI-1和CMERI-2)用于水介质中甲醛(FA)的高效检测。使用高通量溶剂热程序进行明智的溶剂筛选会产生两种具有不同结构的完全不同的金属-有机骨架(MOF)。我们认为CMERI-1框架在FA检测领域显示出更好的灵敏度,响应时间很短(1分钟),这是因为它具有简单的亚胺(?N═(?)形成,这在CMERI-2的情况下受到限制。荧光“开启”行为归因于光诱导电子转移(PET)(从胺亚单位到二级结构单元)过程的抑制。发现CMERI-1和CMERI-2在水介质中对FA的检测限分别为0.62μM(0.019 ppm)和1.39μM(0.041 ppm),远低于细胞内甲醛浓度(100–400μM)。此外,还制备了基于MOF的水凝胶膜,显示了FA的气相检测,这是迄今为止该领域尚未探索的。此外,密度泛函理论(DFT)和Fukui指数分析支持MOF的响应机制。多孔框架的高稳定性及其有趣的传感特性,如快速识别现象、可观的检测限等,促使我们探索其在各种食品样品和水分析中的实际适用性。鉴于我们的聚合物探针的模块化设计原理,所提出的方法可以为构建用于超分子和分析化学领域其他工业污染物的超快检测的强大传感材料开辟新的前景。

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