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Open AccessJournal ArticleDOI

Photo-biocatalytic Cascades: Combining Chemical and Enzymatic Transformations Fueled by Light.

Fatma Feyza Özgen, +2 more
- 02 Mar 2021 - 
- Vol. 22, Iss: 5, pp 790-806
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TLDR
This review highlights general concepts in photo‐biocatalysis, gives various examples of photo‐chemoenzymatic (PCE) cascades, further summarize current synthetic examples of PCE cascades and discusses strategies to address the limitations.
Abstract
In the field of green chemistry, light - an attractive natural agent - has received particular attention for driving biocatalytic reactions. Moreover, the implementation of light to drive (chemo)enzymatic cascade reactions opens up a golden window of opportunities. However, there are limitations to many current examples, mostly associated with incompatibility between the enzyme and the photocatalyst. Additionally, the formation of reactive radicals upon illumination and the loss of catalytic activities in the presence of required additives are common observations. As outlined in this review, the main question is how to overcome current challenges to the exploitation of light to drive (chemo)enzymatic transformations. First, we highlight general concepts in photo-biocatalysis, then give various examples of photo-chemoenzymatic (PCE) cascades, further summarize current synthetic examples of PCE cascades and discuss strategies to address the limitations.

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Citations
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Recent trends in biocatalysis

TL;DR: The research of biocatalysis is gradually moving towards the era of novel technology integration, intelligent manufacturing and enzymatic total synthesis, and gradually complements the lack of remaining key steps in the pathway design of enzyme total synthesis.

Selective sp3 C–H aerobic oxidation enabled by decatungstate photocatalysis in flow

TL;DR: A mild and selective C(sp3)−H aerobic oxidation enabled by decatungstate photocatalysis has been developed and the reaction can be significantly improved in a microflow reactor enabling the safe use of oxygen and enhanced irradiation of the reaction mixture.
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Multistep enzyme cascades as a route towards green and sustainable pharmaceutical syntheses

TL;DR: A broad variety of enzyme cascades used either in vivo (whole cells) or in vitro (purified enzymes) to specifically target pharmaceutically relevant molecules are outlined, from simple building blocks to complex drugs.
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Shortening Synthetic Routes to Small Molecule Active Pharmaceutical Ingredients Employing Biocatalytic Methods

TL;DR: In this paper, a review of large-scale synthetic routes containing biocatalytic key steps toward >130 APIs of approved drugs and drug candidates are compared with the corresponding chemical protocols.
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Interrogating biological systems using visible-light-powered catalysis

TL;DR: In this article, the authors discuss the therapeutic application of photosensitization and advancements made in developing next-generation catalysts, highlighting emerging uses of photoredox catalytic methods for protein bioconjugation and probing complex cellular environments in living cells.
References
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TL;DR: This Review summarizes dual-catalyst strategies that have been applied to synthetic photochemistry, and focuses upon the cooperative interactions of photocatalysts with redox mediators, Lewis and Brønsted acids, organocatalyst, enzymes, and transition metal complexes.
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TL;DR: It is shown that cadmium sulfide (CdS) nanocrystals can be used to photosensitize the nitrogenase molybdenum-iron (MoFe) protein, where light harvesting replaces ATP hydrolysis to drive the enzymatic reduction of N2 into NH3.
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Recent advances in heterogeneous selective oxidation catalysis for sustainable chemistry

TL;DR: Recent advances in the development of new catalytic materials or novel catalytic systems for challenging oxidation reactions, which are important from the viewpoint of green and sustainable chemistry and still remain challenging, are summarized.
Journal ArticleDOI

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TL;DR: This communication demonstrates the homogeneous hydrogenation of CO(2) to CH(3)OH via cascadeCatalysis via cascade catalysis.
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