Cofactor-independent, photoenzymatic, reductions with water mediated by rGQDs

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 17, 2025

Enzymatic reductions catalyzed by reductases, such as aldo/ketoreductases (AKRs), imine and ene reductases generally depend on the regeneration of nicotinamide cofactors for industrial viability. This usually involves addition a cosubstrate second enzyme, dehydrogenase, e.g. glucose / dehydrogenase. For commercial viability it would be more interesting to use water sacrificial supply necessary hydrogen atoms. is possible using photocatalytic methods involving precious metal, Rh Ru, complexes electron mediators. A problem associated with photobiocatalysis in general weak penetration ultraviolet or visible light biological systems. Here we report unprecedented near infrared (NIR) combination hybrid photoenzyme based IR responsive reductive graphene quantum dots (rGQDs) that are non-toxic AKRs. We envisaged immobilization AKR close proximity rGQDs could enable direct transfer atoms from prochiral ketone substrate without requiring cofactor. To test this hypothesis, immobilized surface cross-linked AKR. The resulting rGQD/AKR photobiocatalyst mediated synthesis pharmaceutical intermediate, (R)-1-[3,5-bis(trifluoromethyl)-phenyl] ethanol ((R)-3,5-BTPE) corresponding ketone, 82% yield > 99.99% ee under 50 mW·cm^{− 2} illumination. work opens new avenues create artificial photoenzymes simplify in vitro biocatalysis coupling renewable solar energy sustainable chemical production. Since accounts about half entire spectrum its efficient utilization crucial applications sunlight. have demonstrated our can effectively utilize catalyze enzymatic reduction ketone. these photobiocatalysts insoluble solids they readily recovered, recycled potentially employed continuous flow operation.

Language: Английский

Single-Layer MnO₂ Nanosheets for Immobilization of Agrobacterium radiobacter Halohydrin Dehalogenase via Adsorption

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 6, 2025

Language: Английский

Trendbericht: Organische Chemie 2025

Nachrichten aus der Chemie, Journal Year: 2025, Volume and Issue: 73(3), P. 40 - 70

Published: Feb. 28, 2025

Abstract Highlights von November 2023 bis 2024: die erste Einelektron‐C–C‐σ‐Bindung und Anti‐Bredt‐Verbindung; gesättigte Heterocyclen elektrochemisch funktionalisieren; Ausrichten diskotischer Flüssigkristalle; enantioselektive Wagner‐Meerwein‐Umlagerung reiner Aliphaten; photokatalytisch Furanen zu Pyrrolen; mit Ammoniak primären Arylaminen; Metallschrott recyceln ionischen Flüssigkeiten; terminale Alkene Ni‐Katalysatoren zum (Z)‐ oder (E)‐Alken isomerisieren;neue Fungizide, Medikamente Alkaloide.