Coordination-driven self-assembly of M3L2 trigonal cages from preorganized metalloligands incorporating octahedral metal centers and fluorescent detection of nitroaromatics.
Coordination-driven self-assembly of M3L2 trigonal cages from preorganized metalloligands incorporating octahedral metal centers and fluorescent detection of nitroaromatics.
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DOI：
10.1021/ic1020719
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发表时间：
2011-02-21
影响因子：
4.6
通讯作者：
Stang PJ
中科院分区：
文献类型：
--
作者：
Wang M;Vajpayee V;Shanmugaraju S;Zheng YR;Zhao Z;Kim H;Mukherjee PS;Chi KW;Stang PJ
设计和制备新的M3 L2三角形笼通过协调驱动的自组装的预组织的金属配体含有八面体铝（III），镓（III），或钌（II）中心。通过使用三位或双核线性金属配体和适当的互补亚基，M3 L2三角双锥和三角棱柱笼自组装在温和的条件下。这些3-D笼，其特征在于与多核NMR光谱（1H和31 P）和高分辨率电子喷雾质谱（HR-ESI-MS）。一个这样的三角棱柱笼，自组装从芳烃钌金属配体的结构，通过单晶X射线晶体学证实。这些棱镜的荧光性质，由于其存在的富电子乙炔基官能团，促使电子物理研究表明，缺电子的硝基芳香族化合物是有效的猝灭剂的笼的发射。从棱镜到硝基芳烃底物的激发态电荷转移可用作开发硝基芳烃选择性和区分性关断荧光传感器的基础。
The design and preparation of novel M3L2 trigonal cages via coordination-driven self-assembly of pre-organized metalloligands containing octahedral aluminum(III), gallium(III), or ruthenium(II) centers is described. By employing tritopic or dinuclear linear metalloligands and appropriate complementary subunits, M3L2 trigonal-bipyramidal and trigonal prismatic cages are self-assembled under mild conditions. These 3-D cages were characterized with multinuclear NMR spectroscopy (1H and 31P) and high-resolution electronic spray mass spectrometry (HR-ESI-MS). The structure of one such trigonal prismatic cage, self-assembled from an arene ruthenium metalloligand, was confirmed via single-crystal X-ray crystallography. The fluorescent nature of these prisms, due to the presence of their electron-rich ethynyl functionalities, prompted photophysical studies which revealed that electron-deficient nitroaromatics are effective quenchers of the cages' emission. Excited state charge transfer from the prisms to the nitroaromatic substrates can be used as the basis for developing selective and discriminatory turn-off fluorescent sensors for nitroaromatics.
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