以苯乙烯为原料合成手性醇的 Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction。

IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
ACS Applied Materials & Interfaces Pub Date : 2024-10-09 Epub Date: 2024-09-24 DOI:10.1021/acsami.4c10461
Weiqi Wang, Yuting Yu, Mengyao Wang, Yangxin Wang, Shanqiu Liu, Jian Xu, Zhiyong Sun
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引用次数: 0

摘要

化学生物催化级联已成为先进合成领域一种前景广阔的方法。然而,如何协调不同催化剂之间不相容的反应条件是一项重大挑战。在这里,我们介绍了一种创新的解决方案,即使用 Janus 纳米二氧化硅颗粒稳定的乳液体系,这种颗粒可作为化学催化剂和生物催化剂在界面上的桥梁。化学催化剂被牢固地固定在疏水性聚合物基质中,确保其停留在有机环境中。同时,含有酶的带负电荷的大肠杆菌细胞被吸引到界面上的水相,促进其最佳定位。我们通过两步级联反应展示了这一系统的功效。首先,使用钯作为化学催化剂将苯乙烯氧化成苯乙酮,与对照系统相比,产率提高了 6 倍。随后,将非手性苯乙酮还原为其手性醇衍生物的产率比对照反应提高了 17 倍。重要的是,我们的系统具有多功能性,可在单个反应和连续反应中使用多种底物。这项工作不仅验证了这一概念,还为化学催化剂和生物催化剂在合成更广泛的高价值化合物方面的整合铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction for the Synthesis of Chiral Alcohols from Styrene.

Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction for the Synthesis of Chiral Alcohols from Styrene.

Chemo-biocatalytic cascades have emerged as a promising approach in the realm of advanced synthesis. However, reconciling the incompatible reaction conditions among distinct catalytic species presents a significant challenge. Herein, we introduce an innovative solution using an emulsion system stabilized by Janus silica nanoparticles, which serve as a bridge for both chemo-catalysts and biocatalysts at the interface. The chemo-catalyst is securely anchored within a hydrophobic polymer matrix, ensuring its residence in an organic environment. Meanwhile, the negatively charged E. coli cells containing enzymes are attracted to the aqueous phase at the interface, facilitating their optimal positioning. We demonstrate the efficacy of this system through a two-step cascade reaction. Initially, the oxidation of styrene to acetophenone using palladium as a chemocatalyst achieves a 6-fold increase in yield compared to the control system. Subsequently, the reduction of achiral acetophenone to its chiral alcohol derivative presents a 17-fold yield enhancement relative to that of the control reaction. Importantly, our system exhibits versatility, accommodating a wide range of substrates for both individual and sequential reactions. This work not only validates the concept but also paves the way for the integration of chemo- and biocatalysts in the synthesis of a broader array of high-value chemical compounds.

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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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