Hao Ruipeng, Zhang Ming, Tian Danping, Lei Fu, Qin Zhiqin, Wu Tao, Yang Hengquan
Shanxi Key Laboratory of Coal-based Value-added Chemicals Green Catalysis Synthesis, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China.
College of Chemistry and Materials Science, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, China.
J Am Chem Soc. 2023 Sep 20;145(37):20319-20327. doi: 10.1021/jacs.3c04886. Epub 2023 Sep 7.
The bottom-up assembly of biomimetic multicompartmentalized microreactors for use in continuous flow catalysis remains a grand challenge because of the structural instability or the absence of liquid microenvironments to host biocatalysts in the existing systems. Here, we address this challenge using a strategy that combines stepwise Pickering emulsification with interface-confined cross-linking. Our strategy allows for the fabrication of robust multicompartmentalized liquid-containing microreactors (MLMs), whose interior architectures can be exquisitely tuned in a bottom-up fashion. With this strategy, enzymes and metal catalysts can be separately confined in distinct subcompartments of MLMs for processing biocatalysis or chemo-enzymatic cascade reactions. As exemplified by the enzyme-catalyzed kinetic resolution of racemic alcohols, our systems exhibit a durability of 2000 h with 99% enantioselectivity. Another Pd-enzyme-cocatalyzed dynamic kinetic resolution of amines further demonstrates the versatility and long-term operational stability of our MLMs in continuous flow cascade catalysis. This study opens up a new way to design efficient biomimetic multicompartmental microreactors for practical applications.
由于现有系统中存在结构不稳定性或缺乏容纳生物催化剂的液体微环境，用于连续流动催化的仿生多隔室微反应器的自下而上组装仍然是一个巨大的挑战。在此，我们采用一种将逐步Pickering乳化与界面受限交联相结合的策略来应对这一挑战。我们的策略能够制造出坚固的含多隔室液体微反应器（MLM），其内部结构可以以自下而上的方式进行精确调整。通过这种策略，酶和金属催化剂可以分别被限制在MLM的不同子隔室中，用于进行生物催化或化学酶级联反应。以外消旋醇的酶催化动力学拆分为例，我们的系统在99%对映体选择性下表现出2000小时的耐久性。另一个钯 - 酶共催化的胺动态动力学拆分进一步证明了我们的MLM在连续流动级联催化中的多功能性和长期操作稳定性。这项研究为设计用于实际应用的高效仿生多隔室微反应器开辟了一条新途径。
