Key Laboratory of Carbohydrate Chemistry and Biotechnology, Ministry of Education, School of Biotechnology, Jiangnan University, Wuxi, 214122, P. R. China.
State Key laboratory of Phytochemistry and Plant Resources in West China, Kunming Institute of Botany, Chinese Academy of Sciences, Kunming, 650201, P. R. China.
Angew Chem Int Ed Engl. 2022 Sep 12;61(37):e202208772. doi: 10.1002/anie.202208772. Epub 2022 Aug 4.
This study used light-mediated comparative transcriptomics to identify the biosynthetic gene cluster of beticolin 1 in Cercospora. It contains an anthraquinone moiety and an unusual halogenated xanthone moiety connected by a bicyclo[3.2.2]nonane. During elucidation of the biosynthetic pathway of beticolin 1, a novel non-heme iron oxygenase BTG13 responsible for anthraquinone ring cleavage was discovered. More importantly, the discovery of non-heme iron oxygenase BTG13 is well supported by experimental evidence: (i) crystal structure and the inductively coupled plasma mass spectrometry revealed that its reactive site is built by an atypical iron ion coordination, where the iron ion is uncommonly coordinated by four histidine residues, an unusual carboxylated-lysine (Kcx377) and water; (ii) Kcx377 is mediated by His58 and Thr299 to modulate the catalytic activity of BTG13. Therefore, we believed this study updates our knowledge of metalloenzymes.
本研究利用光介导的比较转录组学方法鉴定了链格孢菌中贝替考林 1 的生物合成基因簇。它含有蒽醌部分和不常见的卤化酮部分，通过双环[3.2.2]壬烷连接。在阐明贝替考林 1 的生物合成途径时，发现了一种新型非血红素铁加氧酶 BTG13，负责蒽醌环裂解。更重要的是，非血红素铁加氧酶 BTG13 的发现得到了实验证据的很好支持：（i）晶体结构和电感耦合等离子体质谱揭示其反应位点由非典型的铁离子配位构建，其中铁离子异常地由四个组氨酸残基、不常见的羧化赖氨酸（Kcx377）和水配位；（ii）Kcx377 由 His58 和 Thr299 介导，调节 BTG13 的催化活性。因此，我们相信这项研究更新了我们对金属酶的认识。
