Multifunctional Integrated Compartment Systems for Incompatible Cascade Reactions Based on Onion-Like Photonic Spheres,Journal of the American Chemical Society

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Multifunctional Integrated Compartment Systems for Incompatible Cascade Reactions Based on Onion-Like Photonic Spheres
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-27 , DOI: 10.1021/jacs.0c00513
Kang Zhou ₁ , Tian Tian ₁ , Chen Wang ₂ , Hongwei Zhao ₁ , Ning Gao ₁ , Hang Yin ₁ , Peng Wang ₁ , Bart Jan Ravoo ₃ , Guangtao Li ₁

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One of the central aims of synthetic biology and metabolic engineering is to mimic the integrality of eukaryotic cells to construct a multifunctional compartment system to perform multistep incompatible cascade reactions in a one-pot, controlled, and selective fashion. The key challenge is how to address the coexistence of antagonistic reagents and to incorporate these functionalities into an integrated system in a smart and efficient way. A novel strategy called "iterative etching-grafting" is proposed here based on monodispersed photonic spheres (PSs) prepared by microfluidics, which constructs a universal platform for incompatible cascade reactions. As a proof of concept, we spatiotemporally regulated the degree of etching of PSs, then grafted precursory groups of acid and base onto PSs, and incorporated a photocleavage method, which were capable of compartmentalizing the acid and base inside PSs. Utilizing the band-gap offsets of PSs could track the progress of cascade reactions in situ, and grafting various charged polymers on the surface of the pores by surface-initiated atom transfer radical polymerization (SI-ATRP) achieved the selectivity of the substrates, which flexibly constructed a multifunctional and integrated acid-base photonic multicompartment system (PMCS). The created PMCS shows excellent catalytic performance, convenient monitoring, and efficient substrate selectivity in the deacetalization-Knoevenagel cascade reaction. Furthermore, two types of electrophile/nucleophile PMCSs have also been accessibly constructed, demonstrating the facile generation of other incompatible systems with the versatility as well as the advancement and extensibility of the developed strategy.

中文翻译：

基于洋葱状光子球的不相容级联反应多功能集成隔室系统

合成生物学和代谢工程的中心目标之一是模拟真核细胞的完整性，以构建多功能区室系统，以一锅、受控和选择性的方式执行多步不相容的级联反应。关键挑战是如何解决拮抗剂的共存问题，并以智能高效的方式将这些功能整合到一个集成系统中。基于微流体制备的单分散光子球 (PSs)，这里提出了一种称为“迭代蚀刻接枝”的新策略，该策略构建了不相容级联反应的通用平台。作为概念证明，我们在时空上调节 PSs 的蚀刻程度，然后将酸和碱的前体基团接枝到 PSs 上，并结合光裂解方法，能够将 PS 内的酸和碱区分开来。利用 PSs 的带隙偏移量可以原位跟踪级联反应的进程，并通过表面引发的原子转移自由基聚合 (SI-ATRP) 在孔表面接枝各种带电聚合物，实现了底物的选择性。灵活构建了多功能集成酸碱光子多室系统（PMCS）。所创建的 PMCS 在脱缩醛-Knoevenagel 级联反应中显示出优异的催化性能、方便的监测和有效的底物选择性。此外，还构建了两种类型的亲电/亲核 PMCS，

更新日期：2020-11-27

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