Abstract
The biosynthetic gene cluster responsible for the production of C2-asymmetric 16-membered dilactones, including pyrenophorol and its derivatives, was discovered through genome mining of polyketides from a sponge-derived fungus. The biosynthetic pathway of the pyrenophorol dilactones was subsequently elucidated. A distinctive flavoenzyme PylE was identified to catalyze the isomerization of the 4-alcohol-2,3-unsaturated moiety within the dilactone scaffold, resulting in the formation of a 1,4-diketone. Further insights into the catalytic mechanism of PylE were obtained through mutagenesis experiments combined with molecular docking.
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