Roy J. Carver Department of Biochemistry, Biophysics & Molecular Biology, Iowa State University , Ames, Iowa 50011, United States.
Department of Chemistry, University of California , Davis, California 95616, United States.
Org Lett. 2018 Feb 16;20(4):1200-1202. doi: 10.1021/acs.orglett.8b00121. Epub 2018 Feb 1.
Biosynthesis of the complex diterpenoid antibiotic pleuromutilin relies on a bifunctional (di)terpene synthase, and here site-directed mutagenesis was used to knockout either of the two active sites. This enabled characterization of the novel ring contracted intermediate produced by the initiating class II diterpene cyclase active site. Quantum chemical calculations further indicate the importance of reactant configuration for this intriguing ring rearrangement.
复杂二萜抗生素雷帕霉素的生物合成依赖于一种双功能（二）萜烯合酶，在这里，定点突变被用来敲除两个活性位点中的任何一个。这使得能够对新型的环缩合中间产物进行表征，该中间产物是由起始的 II 类二萜环化酶活性位点产生的。量子化学计算进一步表明反应物构型对于这种有趣的环重排反应的重要性。
