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Light-driven Enzymatic Decarboxylation
Published on: May 22, 2016
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Photobiocatalysis for Abiological Transformations
Wesley Harrison1,2, Xiaoqiang Huang1,2, Huimin Zhao1,2,3
1Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, 600 S. Matthews Avenue, Urbana, Illinois 61801, United States.
Accounts of Chemical Research
|March 30, 2022
Summary
Combining biocatalysis and photocatalysis creates novel synthetic methods for greener chemistry. This research explores new strategies to expand photobiocatalysis applications, enabling selective, non-natural transformations with high efficiency.
Area of Science:
- Synthetic Chemistry
- Biocatalysis
- Photocatalysis
Background:
- Biocatalysis and photocatalysis are powerful tools in synthetic chemistry.
- Combining these fields offers advantages like high selectivity, enantioselectivity, and greener processes.
- Enzymes can be engineered to control reactive intermediates, enhancing chemo- and stereoselectivity.
Purpose of the Study:
- To explore novel synthetic methodologies by combining photocatalysis and biocatalysis.
- To introduce non-natural reactivity into enzymes through strategic combinations.
- To expand the applications of photobiocatalysis for solving synthetic organic chemistry challenges.
Main Methods:
- Developing synergistic cooperative stereoconvergent reduction systems.
- Utilizing photosensitized energy transfer with ene-reductase-catalyzed reactions.
- Employing cofactor-dependent photoenzymatic systems for enantioselective radical hydroalkylations.
- Irradiating electron donor-acceptor complexes with unnatural substrates.
Main Results:
- Demonstrated a cooperative system for stereoconvergent alkene reduction.
- Enabled enantioselective bimolecular radical hydroalkylations using photoenzymatic systems.
- Showcased strategies including repurposing photoenzymes, elucidating new photoreactivity, combining external photocatalysts with enzymes, and constructing artificial photoenzymes.
Conclusions:
- The combination of biocatalysis and photocatalysis unlocks new-to-nature chemistry.
- Strategic approaches can introduce non-natural reactivity into enzymes.
- Photobiocatalysis offers a promising solution for complex synthetic challenges.
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