Takashima Yohei, Martínez Virginia Martínez, Furukawa Shuhei, Kondo Mio, Shimomura Satoru, Uehara Hiromitsu, Nakahama Masashi, Sugimoto Kunihisa, Kitagawa Susumu
1] ERATO Kitagawa Integrated Pores Project, Japan Science and Technology Agency (JST), Kyoto Research Park Building no. 3, Shimogyo-ku, Kyoto 600-8815, Japan. [2] Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan.
Nat Commun. 2011 Jan 25;2:168. doi: 10.1038/ncomms1170.
Chemosensors detect a single target molecule from among several molecules, but cannot differentiate targets from one another. In this study, we report a molecular decoding strategy in which a single host domain accommodates a class of molecules and distinguishes between them with a corresponding readout. We synthesized the decoding host by embedding naphthalenediimide into the scaffold of an entangled porous framework that exhibited structural dynamics due to the dislocation of two chemically non-interconnected frameworks. An intense turn-on emission was observed on incorporation of a class of aromatic compounds, and the resulting luminescent colour was dependent on the chemical substituent of the aromatic guest. This unprecedented chemoresponsive, multicolour luminescence originates from an enhanced naphthalenediimide-aromatic guest interaction because of the induced-fit structural transformation of the entangled framework. We demonstrate that the cooperative structural transition in mesoscopic crystal domains results in a nonlinear sensor response to the guest concentration.
化学传感器能够从多个分子中检测出单个目标分子，但无法区分不同的目标分子。在本研究中，我们报告了一种分子解码策略，其中单个主体域容纳一类分子，并通过相应的读出方式对它们进行区分。我们通过将萘二酰亚胺嵌入到一个缠结多孔框架的支架中来合成解码主体，该框架由于两个化学上不相连的框架的位错而表现出结构动力学。在加入一类芳香族化合物时观察到强烈的开启发射，并且所产生的发光颜色取决于芳香族客体的化学取代基。这种前所未有的化学响应性多色发光源于缠结框架的诱导契合结构转变导致的萘二酰亚胺 - 芳香族客体相互作用增强。我们证明介观晶域中的协同结构转变导致对客体浓度的非线性传感器响应。
