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Researchers discovered novel natural products by exploring fungal biosynthetic pathways lacking known enzymes. They identified a new enzyme, arginine-containing cyclodipeptide synthase (RCDPS), responsible for creating unique cyclo-arginine dipeptides.

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Area of Science:

  • Natural Product Discovery
  • Biochemistry
  • Molecular Biology

Background:

  • Genome mining enables the discovery of natural products with unknown biosynthetic routes and structures.
  • Conserved fungal pathways often lack identifiable core enzymes, presenting a challenge for natural product identification.

Purpose of the Study:

  • To identify the natural product and biosynthetic pathway associated with a conserved fungal pathway lacking a canonical core enzyme.
  • To characterize the newly identified enzyme and its role in synthesizing novel compounds.

Main Methods:

  • Genome mining of fungal DNA.
  • Heterologous expression of the identified biosynthetic pathway in a model organism.
  • Biochemical characterization of the enzyme and its products.
  • Aminoacyl-tRNA dependency assays.

Main Results:

  • Discovery of a highly modified cyclo-arginine-tyrosine dipeptide.
  • Identification and characterization of a novel arginine-containing cyclodipeptide synthase (RCDPS), unrelated to known peptide synthetases.
  • Demonstration that RCDPS homologs can synthesize diverse cyclo-arginine dipeptides.
  • Confirmation of aminoacyl-tRNA dependency for RCDPS activity using a cyclo-arginine-tryptophan synthesizing enzyme.

Conclusions:

  • The study reveals a new class of enzymes (RCDPS) involved in fungal natural product biosynthesis.
  • This discovery expands the known repertoire of cyclodipeptide synthases and their mechanisms.
  • The findings facilitate the prediction and discovery of new natural products with complex structures.