Abstract
Fungal alkylresorcinols are a class of polyketides,which are commonly synthesized by the hybridization of highly reducing polyketide synthase(hrPKS)with non-reducing polyketide synthase(nrPKS).In this study,we identified and demonstrated a new assembly model for synthesizing alkylresorcinol(scirpilin A,1),which was accomplished by collaboration of a hrPKS(FscA)and a type Ⅲ PKS(FscB).Furthermore,three post-tailoring enzymes(FscC,FscD,and FscE)act iteratively on 1 skeleton,including successive 14e-oxidation of inert carbons,di-halogenation,and di-methylation,to form highly oxidized and multi-substituted alkylresorcinols.Our work presents an unusual synthesis manner of alkylresorcinols,sheds light on the collaborative mechanism between hrPKS and type Ⅲ PKS and provides three valuable enzy-matic catalysts for the tailoring of alkylresorcinol family natural products in future.
基金项目
National Natural Science Foundation of China(22277100)
National Key R&D Program of China(2020YFA0907700)
Fundamental Research Funds for the Central Universities(SWU-KQ22034)
Fundamental Research Funds for the Central Universities(SWU-XDPY22009)
Science and Technology Innovation Key R&D Program of Chongqing(CSTB2022TIAD-STX0015)
Chongqing Science Funds for Distinguished Young Scientists(cstc2020jcyjjqX0005)
万方数据