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作为高效催化和多功能发光传感平台的一系列热调制有机框架材料

Series of TM-OFs as a Platform for Efficient Catalysis and Multifunctional Luminescence Sensing.

作者信息

Liu Yang, Liu Hongyan, Shi Xiaolei, Yan Hui, Guo Wenxiao, Wang Shufang, Ma Xiaoxue, Zhang Lu, Kong Lingqian, Chen Guifang, Ju Xiuping, Li Xia, Yang Yan, Zhu Hongjie, Li Yunwu, Dai Fangna, Hao Hongguo

机构信息

Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry and Chemical Engineering, School of Pharmacy, and Dongchang College, Liaocheng University, Liaocheng 252059, People's Republic of China.

College of Science, School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao, Shandong 266580, People's Republic of China.

出版信息

Inorg Chem. 2022 Oct 10;61(40):15880-15894. doi: 10.1021/acs.inorgchem.2c01848. Epub 2022 Sep 25.

DOI:10.1021/acs.inorgchem.2c01848
PMID:36154014
Abstract

Three novel porous transition-metal-organic frameworks (TM-OFs), formulated as Co(DCPN)(μ-OH)(HO) (), Cd(DCPN)(μ-OH)(HO) (), and [CdK(DCPN)(DMA)] (), have been successfully prepared via solvothermal conditions based on a 5-(3',6'-dicarboxylic phenyl) nicotinic carboxylic acid (HDCPN) ligand. and both have the same porous 3D network structure with the point symbol of {4·6·8}·{4·6} based on trinuclear ({Co} or {Cd}) clusters, indicating a one-dimensional porous channel, and possess excellent water and thermal stability; also displays a porous 3D network structure with a 4-connected topology based on the heteronuclear metal cluster {CdK}. Complex can be used to load Pd nanoparticles (Pd NPs) via a wetness impregnation strategy to obtain Pd@. The reduction of nitrophenols (2-NP, 3-NP, 4-NP) by Pd@ in aqueous solution shows outstanding conversion, excellent rate constants (), and remarkable cycling stability due to the synergistic effect of complex and Pd NPs. Luminescence sensing tests confirmed that is a reliable multifunctional chemical sensor with high selectivity and sensitivity for low concentrations of Fe, CrO, CPFX, and NFX. Specifically, shows a fluorescence enhancement behavior toward fluoroquinolone antibiotics (CPFX and NFX), which has not been reported previously in the literature. Moreover, the rational mechanism of fluorescence sensing was also systematically investigated by various detection means and theoretical calculations.

摘要

基于5-(3',6'-二羧酸苯基)烟酸(HDCPN)配体,通过溶剂热条件成功制备了三种新型多孔过渡金属有机框架(TM-OFs),分别为[Co(DCPN)(μ-OH)(H₂O)]·(DMF)()、[Cd(DCPN)(μ-OH)(H₂O)]·(DMF)()和[CdK(DCPN)(DMA)]()。和都具有相同的多孔三维网络结构,基于三核({Co}或{Cd})簇的点符号为{4·6·8}·{4·6},表明存在一维多孔通道,并且具有优异的水稳定性和热稳定性;基于异核金属簇{CdK},还展示了具有4连接拓扑结构的多孔三维网络结构。配合物可通过湿浸渍策略用于负载钯纳米颗粒(Pd NPs)以获得Pd@。由于配合物和Pd NPs的协同作用,Pd@在水溶液中对硝基苯酚(2-NP、3-NP、4-NP)的还原显示出出色的转化率、优异的速率常数()和显著的循环稳定性。发光传感测试证实,是一种可靠的多功能化学传感器,对低浓度的Fe、CrO₄²⁻、CPFX和NFX具有高选择性和灵敏度。具体而言,对氟喹诺酮类抗生素(CPFX和NFX)表现出荧光增强行为,这在以前的文献中尚未报道。此外,还通过各种检测手段和理论计算系统地研究了荧光传感的合理机制。

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