期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 103, 期 24, 页码 8977-8982出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0603148103
关键词
mass spectrometry; orphan gene cluster; hybrid nonribosomal peptide/polyketide; polyketide methylation
资金
- NIGMS NIH HHS [F32 GM073323, R01 GM067725, R01 GM049338, GM 067725, GM 49338, F32 GM 073323-01] Funding Source: Medline
The pksX gene cluster from Bacillus subtilis is predicted to encode the biosynthesis of an as yet uncharacterized hybrid nonribosomal pepticle/polyketide secondary metabolite. We used a combination of biochemical and mass spectrometric techniques to assign functional roles to the proteins AcpK, PksC, PksL, PksF, PksG, PksH, and PksI, and we conclude that they act to incorporate an acetate-derived P-methyl branch on an acetoacetyl-S-carrier protein and ultimately generate a Delta(2)-isoprenyi-S-carrier protein. This work highlights the power of mass spectrometry to elucidate the functions of orphan biosynthetic enzymes, and it details a mechanism by which single-carbon ss-branches can be inserted into polyketide-like structures. This pathway represents a noncanonical route to the construction of prenyl units and serves as a prototype for the intersection of isoprenoid and polyketide biosynthetic manifolds in other natural product biosynthetic pathways.
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