TY - JOUR
T1 - Cofactor-independent photo-enzymatic reductions with water mediated by reductive graphene quantum dots
AU - Wang, Anming
AU - Li, Xiaoyu
AU - Qiao, Li
AU - Pan, Xiaoting
AU - Jiang, Yongjian
AU - Wang, Zhiguo
AU - Ye, Wei
AU - Gao, Peng
AU - Sheldon, Roger A.
PY - 2025
Y1 - 2025
N2 - Enzymatic reductions catalyzed by reductases generally depend on reduced nicotinamide cofactors as a hydride source. However, for industrial viability, it is more cost-effective to use water as the hydrogen source, bypassing the requirement for the cofactor. Here we report a hybrid photo-biocatalyst system based on infrared (IR) light and responsive reductive graphene quantum dots (rGQDs), for performing the direct transfer of hydrogen from water to prochiral substrates. The photo-biocatalyst, assembled from rGQDs and cross-linked aldo-keto reductase (AKR), mediates the synthesis of the pharmaceutical intermediate, (R)−1-[3,5-bis(trifluoromethyl)-phenyl] ethanol ((R)−3,5-BTPE), in 82% yield and >99.99% ee under IR illumination. Our photo-enzymatic systems can also be effectively used to drive the enzymatic reduction of imines and alkenes. Since the hybrid photo-biocatalysts are insoluble, they can be readily recovered and recycled. This work opens new avenues to create artificial photo-biocatalyst systems, enabling the facile coupling of renewable solar energy and sustainable chemical production.
AB - Enzymatic reductions catalyzed by reductases generally depend on reduced nicotinamide cofactors as a hydride source. However, for industrial viability, it is more cost-effective to use water as the hydrogen source, bypassing the requirement for the cofactor. Here we report a hybrid photo-biocatalyst system based on infrared (IR) light and responsive reductive graphene quantum dots (rGQDs), for performing the direct transfer of hydrogen from water to prochiral substrates. The photo-biocatalyst, assembled from rGQDs and cross-linked aldo-keto reductase (AKR), mediates the synthesis of the pharmaceutical intermediate, (R)−1-[3,5-bis(trifluoromethyl)-phenyl] ethanol ((R)−3,5-BTPE), in 82% yield and >99.99% ee under IR illumination. Our photo-enzymatic systems can also be effectively used to drive the enzymatic reduction of imines and alkenes. Since the hybrid photo-biocatalysts are insoluble, they can be readily recovered and recycled. This work opens new avenues to create artificial photo-biocatalyst systems, enabling the facile coupling of renewable solar energy and sustainable chemical production.
UR - http://www.scopus.com/inward/record.url?scp=105016666930&partnerID=8YFLogxK
U2 - 10.1038/s41467-025-61908-6
DO - 10.1038/s41467-025-61908-6
M3 - Article
C2 - 40962842
AN - SCOPUS:105016666930
SN - 2041-1723
VL - 16
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 8310
ER -
