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将脂质体光催化剂与全细胞催化剂相结合用于一锅法光生物催化。

Combining Liposomal Photocatalysts with Whole-Cell Catalysts for One-pot Photobiocatalysis.

作者信息

Zhang Jiaheng, Batista Vasco F, Hübner René, Vogel Stefan, Wu Changzhu

机构信息

Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Campusvej 55, Odense, 5230, Denmark.

Helmholtz-Zentrum Dresden - Rossendorf (HZDR), Institute of Ion Beam Physics and Materials Research, Bautzner Landstrasse 400, 01328, Dresden, Germany.

出版信息

Small. 2024 Dec 1:e2408666. doi: 10.1002/smll.202408666.

Abstract

Cooperative photobiocatalytic processes have seen extensive potentials for the synthesis of both bulk and fine chemicals owing to their versatility, eco-friendliness, and cost-effectiveness. Nevertheless, developing a universal and effective synthetic strategy compatible with both catalytic systems remains challenging. In this study, we explored cationic liposomes as biocompatible photocatalyst encapsulation systems and combined them with bacteria overexpressing enzymes for two-step and three-step cascade reactions. Specifically, the water-soluble photocatalyst anthraquinone-2-sulfonate (AQS), which can oxidize benzyl alcohol, is encapsulated within the core of cationic liposomes composed of dioleoyl-3-trimethylammonium propane (DOTAP) and the helper lipid cholesterol. The positive charge on the liposome surface enabled electrostatic interactions with the negative charges on the membrane of Escherichia coli cells. Bacterial cells overexpressing various enzymes, such as Candida antarctica lipase B (CalB) and benzaldehyde lyase (BAL), and coated with liposomes enabled the production of added value compounds through cascade reactions with excellent production. These cascades involve CalB-catalyzed hydrolysis, BAL-catalyzed condensation, and AQS-driven photo-oxidation reactions. Therefore, the strategy offers more possibilities of combining photocatalysis with biocatalysis for recoverability, enhanced mass transfer, and enhanced compatibility in both industrial biotechnology and synthetic chemistry.

摘要

由于其多功能性、生态友好性和成本效益,合作光生物催化过程在大宗化学品和精细化学品的合成方面具有广泛的潜力。然而,开发一种与两种催化系统兼容的通用且有效的合成策略仍然具有挑战性。在本研究中,我们探索了阳离子脂质体作为生物相容性光催化剂封装系统,并将它们与过表达酶的细菌相结合用于两步和三步级联反应。具体而言,可氧化苯甲醇的水溶性光催化剂蒽醌 - 2 - 磺酸盐(AQS)被封装在由二油酰基 - 3 - 三甲基铵丙烷(DOTAP)和辅助脂质胆固醇组成的阳离子脂质体核心内。脂质体表面的正电荷使其能够与大肠杆菌细胞膜上的负电荷发生静电相互作用。过表达各种酶(如南极假丝酵母脂肪酶B(CalB)和苯甲醛裂解酶(BAL))并包被有脂质体的细菌细胞能够通过级联反应以优异的产量生产增值化合物。这些级联反应包括CalB催化的水解、BAL催化的缩合以及AQS驱动的光氧化反应。因此,该策略为光催化与生物催化的结合提供了更多可能性,以实现工业生物技术和合成化学中的可回收性、增强的传质以及增强的兼容性。

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