State Key Laboratory of Structural Chemistry , Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences , Fuzhou 350002 , China.
University of Chinese Academy of Sciences , Beijing 100049 , China.
J Am Chem Soc. 2019 Oct 16;141(41):16344-16353. doi: 10.1021/jacs.9b07175. Epub 2019 Oct 4.
Molecular switches are an intensive area of research, and in particular, the control of multistate switching is challenging. Herein we introduce a general and versatile strategy of dynamic covalent switches and communicating networks, wherein distinct states of reversible covalent systems can induce addressable fluorescence switching. The regulation of intramolecular ring/chain equilibrium, intermolecular dynamic covalent reactions (DCRs) with amines, and both permitted the activation of optical switches. The variation in electron-withdrawing competition between the fluorophore and 2-formylbenzenesulfonyl unit afforded diverse signaling patterns. The combination of switches further enabled the creation of communicating networks for multistate color switching, including white emission, through the delicate control of DCRs in complex mixtures. Finally, reversible and recyclable multiresponsive luminescent materials were achieved with molecular networks on the solid support, allowing visualization of different types of vapors and quantification of primary amine vapors with high sensitivity and wide detection range. The results reported herein should be appealing for future studies of dynamic assemblies, molecular sensing, intelligent materials, and biological labeling.
分子开关是一个研究热点,特别是多态开关的控制极具挑战性。在此,我们介绍了一种通用的动态共价开关和通信网络的策略,其中可逆共价体系的不同状态可以诱导可寻址的荧光开关。分子内环/链平衡的调控、与胺的分子间动态共价反应(DCR)以及二者都允许光学开关的激活。荧光团和 2-甲酰基苯磺酰基单元之间的吸电子竞争的变化提供了多样化的信号模式。通过在复杂混合物中精细控制 DCR,开关的组合进一步实现了用于多态颜色切换的通信网络,包括白色发射。最后,通过在固体载体上的分子网络实现了可逆和可回收的多响应发光材料,允许可视化不同类型的蒸气并以高灵敏度和宽检测范围定量检测伯胺蒸气。本文报道的结果对于动态组装、分子传感、智能材料和生物标记的未来研究应该具有吸引力。