来自Lentzea atacamensis的两个sesterterpene合成表明了基生物合成中形状变化的作用
Binbin Gu1, Bernd Goldfuss2, Jeroen S Dickschat1
1Kekulé-Institute for Organic Chemistry and Biochemistry, University of Bonn, Gerhard-Domagk-Straße 1, 53121, Bonn, Germany.
Angewandte Chemie (International ed. in English)
|February 19, 2024
概括
研究人员从Lentzea atacamensis中确定了两种新的烯合成酶,产生了新型化合物,并揭示了基质灵活性对于烯循环化至关重要. 这项工作突出了生物合成期间酶活性位点的构造变化.
科学领域:
- 生物化学 生物化学
- 自然产品化学 自然产品化学
- 酶学 是一种酶学.
背景情况:
- 类是具有显著生物活动的多样化的自然产品类别.
- 聚合成酶 (STSs) 是负责聚的生物合成的酶,这是一个较少探索的类的子类.
- 了解STS的机制对于发现新的化合物和生物合成途径至关重要.
研究的目的:
- 鉴定和描述来自Lentzea atacamensis细菌的两个多产品甲合成酶LaLDS和LaATS.
- 阐明这些酶所采用的生物合成途径和机制.
- 调查基质结构灵活性在烯循环中的作用.
主要方法:
- 基因挖掘和特合成酶的异质表达.
- 用LC-MS/MS和NMR进行酶活性和产品分析的生物化学表征.
- 同位素标记实验,以追踪反应机制.
- 密度函数理论 (DFT) 计算以建模反应路径和过渡状态.
主要成果:
- 识别生产泽 (一种新化合物) 和相关的甲的LaLDS.
- 识别LaATS产生六种新的甲化合物,包括Bm1.1的反体.
- 证明两种酶的产品概况都需要格兰二酸盐基质的结构灵活性.
- 在lentzeadiene生物合成中发现了热[1,5]-sigmatropic重组,类似于维生素D3的形成.
结论:
- 兰特西亚阿塔卡门西斯 (Lentzea atacamensis) 拥有独特的甲合成酶,具有广泛的基质接受和复杂的催化机制.
- 基质的形状灵活性对于这些酶形成多种基的形成至关重要.
- 这项研究揭示了新的生物合成途径,并强调了酶基质相互作用在烯循环中的重要性.
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