Functional Characterization of a Ketoreductase-Encoding Gene med-ORF12 Involved in the Formation of a Stereospecific Pyran Ring during the Biosynthesis of an Antitumor Antibiotic Medermycin

PLoS One. 2015 Jul 10;10(7):e0132431. doi: 10.1371/journal.pone.0132431. eCollection 2015.

Abstract

Medermycin, a polyketide antibiotic, possesses strong bioactivity against a variety of tumors through a novel mechanism and is structurally featured with a pyran ring containing two chiral centers (3S and 15R). By far the biosynthetic origin of such enantiomerical conformations still remains obscure. In the present study, we reported the functional characterization of a proposed ketoreductase Med-ORF12 encoded by medermycin biosynthetic cluster and revealed its involvement in the stereochemical control at C3 center of medermycin. Firstly, bioinformatics analysis of Med-ORF12 suggested that it belongs to a group of stereospecific ketoreductases. Next, a Med-ORF12-deficient mutant was obtained and LC/MS measurements demonstrated that medermycin production was completely abolished in this mutant. Meanwhile, it was found that two shunt products were accumulated at the absence of Med-ORF12. Finally, the reintroduction of Med-ORF12 into this mutant could restore the production of medermycin. In a conclusion, these data supported that Med-ORF12 is essential for the biosynthesis of medermycin and performs its role as a stereospecifc ketoreductase in the tailoring steps of medermycin biosynthetic pathway.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Alcohol Oxidoreductases / genetics*
  • Amino Acid Sequence
  • Anthraquinones / metabolism
  • Antibiotics, Antineoplastic / metabolism*
  • Bacterial Proteins / chemistry
  • Biosynthetic Pathways / genetics*
  • Computational Biology
  • Genes, Bacterial*
  • Genetic Complementation Test
  • Metabolomics
  • Molecular Sequence Data
  • Multigene Family
  • Mutation / genetics
  • Naphthoquinones / metabolism
  • Naphthoquinones / pharmacology
  • Open Reading Frames / genetics*
  • Phylogeny
  • Pyrans / metabolism*
  • Sequence Alignment
  • Stereoisomerism
  • Streptomyces / genetics

Substances

  • Anthraquinones
  • Antibiotics, Antineoplastic
  • Bacterial Proteins
  • Naphthoquinones
  • Pyrans
  • medermycin
  • Alcohol Oxidoreductases
  • actinorhodin

Grants and funding

Thanks for financial supports by the National Natural Science Foundation of China (No. 31170050 and 30770036), the Fundamental Research Funds for the Central University (No.CCNU10A02011), and Xinjiang Production & Construction Corps Key Laboratory of Protection and Utilization of Biological Resources in Tarim Basin (No. BRZD1401).