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学科主题: 生命有机化学
题名: Cloning and Elucidation of the FR901464 Gene Cluster Revealing a Complex Acyltransferase-less Polyketide Synthase Using Glycerate as Starter Units
其他题名: 克隆与解析FR901464的生物合成基因簇发现一个复杂的"AT-less"聚酮合酶以甘油为起始单元
作者: Zhang F(张凤) ; He HY(贺海燕) ; Tang MC(唐满成) ; Tang YM(唐玉敏) ; Zhou Q(周强) ; Tang GL(唐功利)
通讯作者: 唐功利
刊名: J. Am. Chem. Soc.
发表日期: 2011
卷: 133, 期:8, 页:2452-2462
收录类别: SCI
部门归属: 中科院上海有机化学研究所
英文摘要: FR901464, an antitumor natural product, represents a new class of potent anticancer small molecules targeting spliceosome and inhibiting both splicing and nuclear retention of pre-mRNA. Herein we describe the biosynthetic gene cluster of FR901464, identified by degenerate primer PCR amplification of a gene encoding the 3-hydroxy-3-methylglutaryl-CoA synthase (HCS) postulated to be involved in the biosynthesis of a beta-branched polyketide from Pseudomonas sp. No. 2663. This cluster consists of twenty open reading frames (ORFs) and was localized to 93-kb DNA segment, and its involvement in FR901464 biosynthesis was confirmed by gene inactivation and complementation. FR901464 is biosynthesized by a hybrid polyketide synthase (PKS)/nonribosomal peptide synthetase (NRPS), HCS, and acyltransferases (AT)-less system. The PKS/NRPS modules feature unusual domain organization including multiple domain redundancy, inactivation, and tandem. Biochemical characterization of a glyceryl transferase and an acyl carrier protein (ACP) in the start module revealed that it incorporates D-1,3-bisphosphoglycerate, which is dephosphorylated and transferred to ACP as the starter unit. Furthermore, an oxidative Baeyer Villiger reaction followed by chain release was postulated to form a pyran moiety. On the basis of in silico analysis and genetic and biochemical evidances, a biosynthetic pathway for FR901464 was proposed, which sets the stage to further investigate the complex PKS biochemically and engineer the biosynthetic machinery for the production of novel analogues.
语种: 英语
相关网址: 查看原文
WOS记录号: WOS:000288291300029
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内容类型: 期刊论文
URI标识: http://ir.sioc.ac.cn/handle/331003/28467
Appears in Collections:生命有机化学国家重点实验室_期刊论文

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Recommended Citation:
Zhang F,He HY,Tang MC,et al. Cloning and Elucidation of the FR901464 Gene Cluster Revealing a Complex Acyltransferase-less Polyketide Synthase Using Glycerate as Starter Units[J]. J. Am. Chem. Soc.,2011,133(8):2452-2462.
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