School of Chemistry and EaStCHEM, University of St Andrews , North Haugh, St Andrews, Fife KY16 9ST, U.K.
J Am Chem Soc. 2016 Jun 1;138(21):6723-6. doi: 10.1021/jacs.6b03372. Epub 2016 May 20.
A simple synthetic autocatalytic replicator is capable of establishing and driving the propagation of a reaction-diffusion front within a 50 μL syringe. This replicator templates its own synthesis through a 1,3-dipolar cycloaddition reaction between a nitrone component, equipped with a 9-ethynylanthracene optical tag, and a maleimide. Kinetic studies using NMR and UV-vis spectroscopies confirm that the replicator forms efficiently and with high diastereoselectivity, and this replication process brings about a dramatic change in optical properties of the sample-a change in the color of the fluorescence in the sample from yellow to blue. The addition of a small amount of the preformed replicator at a specific location within a microsyringe, filled with the reaction building blocks, results in the initiation and propagation of a reaction-diffusion front. The realization of a replicator capable of initiating a reaction-diffusion front provides a platform for the examination of interconnected replicating networks under out-of-equilibrium conditions involving diffusion processes.
一种简单的自催化复制子能够在 50μL 注射器内建立并驱动反应-扩散前沿的传播。该复制子通过氮丙啶组分(带有 9-乙炔基蒽光学标记)和马来酰亚胺之间的 1,3-偶极环加成反应模板其自身的合成。使用 NMR 和 UV-vis 光谱法的动力学研究证实,该复制子有效地形成,具有高非对映选择性,并且该复制过程使样品的光学性质发生显著变化-样品中荧光的颜色从黄色变为蓝色。在充满反应构建块的微注射器的特定位置添加少量预先形成的复制子,可引发并传播反应-扩散前沿。能够引发反应-扩散前沿的复制子的实现为在涉及扩散过程的非平衡条件下检查相互连接的复制网络提供了一个平台。