摘要
We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster,which contains a uniqueα-ketoglutarate-dependent dioxygenase(αKGD)enzyme,AbnI.Our findings revealed that AbnI demonstrates remarkable substrate promiscuity and is capable of activating multiple sites on both 5-8-5 and 5-9-5 brassicicene skeletons,resulting in skeleton modifications and an unexpected ring system rearrangement.These results suggested the potential utility of AbnI as an enzymatic tool for terpene C-H functionalization.In addition,the catalytic mechanism of AbnI and its potential ecological implications were discussed.
基金
financially supported by the National Key R&D Program of China(Nos.2021YFA0910500,2021YFA0910503)
the National Natural Science Foundation of China(Nos.22277035,32000045 and 81973205)
the Program for Changjiang Scholars of Ministry of Education of the People’s Republic of China(No.T2016088)
the National Natural Science Foundation for Distinguished Young Scholars(No.81725021)
the National Science and Technology Project of China(No.2018ZX09201001-001-003)
Innovative Research Groups of the National Natural Science Foundation of China(No.81721005)
the Fundamental Research Funds for the Central Universities(No.2020kfyXJJS043).