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Cofactor-independent photo-enzymatic reductions with water mediated by reductive graphene quantum dots

Author

Listed:
  • Anming Wang

    (Hangzhou Normal University)

  • Xiaoyu Li

    (Hangzhou Normal University)

  • Li Qiao

    (Hangzhou Normal University)

  • Xiaoting Pan

    (Hangzhou Normal University)

  • Yongjian Jiang

    (Hangzhou Normal University)

  • Zhiguo Wang

    (Hangzhou Normal University)

  • Wei Ye

    (Hangzhou Normal University)

  • Peng Gao

    (Hangzhou Normal University
    University of Electronic Science and Technology)

  • Roger A. Sheldon

    (PO Wits.
    Van der Maasweg 9)

Abstract

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.

Suggested Citation

  • Anming Wang & Xiaoyu Li & Li Qiao & Xiaoting Pan & Yongjian Jiang & Zhiguo Wang & Wei Ye & Peng Gao & Roger A. Sheldon, 2025. "Cofactor-independent photo-enzymatic reductions with water mediated by reductive graphene quantum dots," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-61908-6
    DOI: 10.1038/s41467-025-61908-6
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    References listed on IDEAS

    as
    1. Maria Mifsud & Serena Gargiulo & Sara Iborra & Isabel W. C. E. Arends & Frank Hollmann & Avelino Corma, 2014. "Photobiocatalytic chemistry of oxidoreductases using water as the electron donor," Nature Communications, Nature, vol. 5(1), pages 1-6, May.
    2. Benjamin D. Ravetz & Andrew B. Pun & Emily M. Churchill & Daniel N. Congreve & Tomislav Rovis & Luis M. Campos, 2019. "Author Correction: Photoredox catalysis using infrared light via triplet fusion upconversion," Nature, Nature, vol. 570(7759), pages 24-24, June.
    3. Elijah N. Kissman & Max B. Sosa & Douglas C. Millar & Edward J. Koleski & Kershanthen Thevasundaram & Michelle C. Y. Chang, 2024. "Expanding chemistry through in vitro and in vivo biocatalysis," Nature, Nature, vol. 631(8019), pages 37-48, July.
    4. Xiaoqiang Huang & Binju Wang & Yajie Wang & Guangde Jiang & Jianqiang Feng & Huimin Zhao, 2020. "Photoenzymatic enantioselective intermolecular radical hydroalkylation," Nature, Nature, vol. 584(7819), pages 69-74, August.
    5. Megan A. Emmanuel & Norman R. Greenberg & Daniel G. Oblinsky & Todd K. Hyster, 2016. "Accessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light," Nature, Nature, vol. 540(7633), pages 414-417, December.
    6. Long Kuai & Zheng Chen & Shoujie Liu & Erjie Kan & Nan Yu & Yiming Ren & Caihong Fang & Xingyang Li & Yadong Li & Baoyou Geng, 2020. "Titania supported synergistic palladium single atoms and nanoparticles for room temperature ketone and aldehydes hydrogenation," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
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