Journal
CELL CHEMICAL BIOLOGY
Volume 24, Issue 7, Pages 881-891Publisher
CELL PRESS
DOI: 10.1016/j.chembiol.2017.06.008
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Funding
- NSF of China [31370134, 31425001, 31300033, 21661140002]
- MOST [2012CB721000, 2010AA10A201]
- Chinese-Australia Joint Grant [2016YFE0101000]
- US NIH [R01 GM 105977]
- Science and Technology Commission of Shanghai Municipality [15JC1400401]
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Bacterial aromatic polyketides are a group of natural products synthesized by polyketide synthases (PKSs) that show diverse structures and biological activities. They are structurally subclassified into linear, angular, and discoid aromatic polyketides, the formation of which is commonly determined by the shaping and folding of the poly-beta-keto intermediates under the concerted actions of the minimal PKSs, cyclases and ketoreductases. Murayaquinone, found in several streptomycetes, possesses an unusual tricyclic angular aromatic polyketide core containing a 9,10-phenanthraquinone. In this study, genes essential for murayaquinone biosynthesis were identified, and a linear anthraoxirene intermediate was discovered. A unique biosynthetic model for the angular aromatic polyketide formation was discovered and confirmed through in vivo and in vitro studies. Three oxidoreductases, MrqO3, MrqO6, and MrqO7, were identified to catalyze the conversion of the linear aromatic polyketide intermediate into the final angularly arranged framework, which exemplifies a novel strategy for the biosynthesis of angular aromatic polyketides.
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