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Efficient biosynthesis of nucleoside cytokinin angustmycin A containing an unusual sugar system

Author

Listed:
  • Le Yu

    (Wuhan University)

  • Wenting Zhou

    (Wuhan University)

  • Yixuan She

    (Wuhan University)

  • Hongmin Ma

    (Wuhan University)

  • You-Sheng Cai

    (Wuhan University)

  • Ming Jiang

    (Shanghai Jiao Tong University)

  • Zixin Deng

    (Wuhan University
    Shanghai Jiao Tong University)

  • Neil P. J. Price

    (National Center for Agricultural Utilization Research)

  • Wenqing Chen

    (Wuhan University)

Abstract

Angustmycin A has anti-mycobacterial and cytokinin activities, and contains an intriguing structure in which an unusual sugar with C5′-C6′ dehydration is linked to adenine via an N-glycosidic bond. However, the logic underlying the biosynthesis of this molecule has long remained obscure. Here, we address angustmycin A biosynthesis by the full deciphering of its pathway. We demonstrate that AgmD, C, A, E, and B function as d-allulose 6-phosphate 3-epimerase, d-allulose 6-phosphate pyrophosphokinase, adenine phosphoallulosyltransferase, phosphoribohydrolase, and phosphatase, respectively, and that these collaboratively catalyze the relay reactions to biosynthesize angustmycin C. Additionally, we provide evidence that AgmF is a noncanonical dehydratase for the final step to angustmycin A via a self-sufficient strategy for cofactor recycling. Finally, we have reconstituted the entire six-enzyme pathway in vitro and in E. coli leading to angustmycin A production. These results expand the enzymatic repertoire regarding natural product biosynthesis, and also open the way for rational and rapid discovery of other angustmycin related antibiotics.

Suggested Citation

  • Le Yu & Wenting Zhou & Yixuan She & Hongmin Ma & You-Sheng Cai & Ming Jiang & Zixin Deng & Neil P. J. Price & Wenqing Chen, 2021. "Efficient biosynthesis of nucleoside cytokinin angustmycin A containing an unusual sugar system," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26928-y
    DOI: 10.1038/s41467-021-26928-y
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    References listed on IDEAS

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    1. Takashi Kurakawa & Nanae Ueda & Masahiko Maekawa & Kaoru Kobayashi & Mikiko Kojima & Yasuo Nagato & Hitoshi Sakakibara & Junko Kyozuka, 2007. "Direct control of shoot meristem activity by a cytokinin-activating enzyme," Nature, Nature, vol. 445(7128), pages 652-655, February.
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