Zhuang Jiaming, Seçinti Hatice, Zhao Bo, Thayumanavan S
Department of Chemistry, University of Massachusetts Amherst, Amherst, MA, 01003, USA.
Angew Chem Int Ed Engl. 2018 Jun 11;57(24):7111-7115. doi: 10.1002/anie.201803029. Epub 2018 May 15.
We report a new molecular design strategy that allows for the propagation of surface enzymatic events inside a supramolecular assembly for accelerated molecular release. The approach addresses a key shortcoming encountered with many of the currently available enzyme-induced disassembly strategies, which rely on the unimer-aggregate equilibria of amphiphilic assemblies. The enzymatic response of the host to predictably tune the kinetics of guest-molecule release can be programmed by controlling substrate accessibility through electrostatic complexation with a complementary polymer. Accelerated guest release in response to the enzyme is shown to be accomplished by a cooperative mechanism of enzyme-triggered supramolecular host disassembly and host reorganization.
我们报道了一种新的分子设计策略，该策略能够使表面酶促反应在超分子组装体内进行，以加速分子释放。这种方法解决了许多现有酶诱导解聚策略所面临的一个关键缺点，这些策略依赖于两亲性组装体的单体 - 聚集体平衡。通过与互补聚合物进行静电络合来控制底物可及性，可对主体的酶促反应进行编程，从而可预测地调节客体分子释放的动力学。研究表明，响应酶的加速客体释放是通过酶触发的超分子主体解聚和主体重组的协同机制实现的。
