Phylogeny‐guided Characterization of Bacterial Hydrazine Biosynthesis Mediated by Cupin/methionyl tRNA Synthetase‐like Enzymes

  • Kenichi Matsuda
    Faculty of Pharmaceutical Sciences Hokkaido University Kita 12, Nishi 6, Kita-ku Sapporo 060-0812 Japan
  • Yuto Nakahara
    Faculty of Pharmaceutical Sciences Hokkaido University Kita 12, Nishi 6, Kita-ku Sapporo 060-0812 Japan
  • Atina Rizkiya Choirunnisa
    Faculty of Pharmaceutical Sciences Hokkaido University Kita 12, Nishi 6, Kita-ku Sapporo 060-0812 Japan
  • Kuga Arima
    Faculty of Pharmaceutical Sciences Hokkaido University Kita 12, Nishi 6, Kita-ku Sapporo 060-0812 Japan
  • Toshiyuki Wakimoto
    Faculty of Pharmaceutical Sciences Hokkaido University Kita 12, Nishi 6, Kita-ku Sapporo 060-0812 Japan

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<jats:title>Abstract</jats:title><jats:p>Cupin/methionyl‐tRNA synthetase (MetRS)‐like didomain enzymes catalyze nitrogen‐nitrogen (N−N) bond formation between <jats:italic>N</jats:italic>ω‐hydroxylamines and amino acids to generate hydrazines, key biosynthetic intermediates of various natural products containing N−N bonds. While the combination of these two building blocks leads to the creation of diverse hydrazine products, the full extent of their structural diversity remains largely unknown. To explore this, we herein conducted phylogeny‐guided genome‐mining of related hydrazine biosynthetic pathways consisting of two enzymes: flavin‐dependent <jats:italic>N</jats:italic>ω‐hydroxylating monooxygenases (NMOs) that produce <jats:italic>N</jats:italic>ω‐hydroxylamine precursors and cupin/MetRS‐like enzymes that couple the <jats:italic>N</jats:italic>ω‐hydroxylamines with amino acids via N−N bonds. A phylogenetic analysis identified the largely unexplored sequence spaces of these enzyme families. The biochemical characterization of NMOs demonstrated their capabilities to produce various <jats:italic>N</jats:italic>ω‐hydroxylamines, including those previously not known as precursors of N−N bonds. Furthermore, the characterization of cupin/MetRS‐like enzymes identified five new hydrazine products with novel combinations of building blocks, including one containing non‐amino acid building blocks: 1,3‐diaminopropane and putrescine. This study substantially expanded the variety of N−N bond forming pathways mediated by cupin/MetRS‐like enzymes.</jats:p>

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詳細情報 詳細情報について

  • CRID
    1360865815482623744
  • DOI
    10.1002/cbic.202300838
  • ISSN
    14397633
    14394227
  • 資料種別
    journal article
  • データソース種別
    • Crossref
    • KAKEN
    • OpenAIRE

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