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迪特尔合成酶的功能性表征和循环机制,催化类型迪特尔类的骨架形成

Changkang Li¹, Shuai Wang^1,2, Xinxin Yin¹

¹State Key Laboratory of Bioactive Substance and Function of Natural Medicines, CAMS Key Laboratory of Enzyme and Biocatalysis of Natural Drugs, NHC Key Laboratory of Biosynthesis of Natural Products, and Beijing Key Laboratory of Non-Clinical Drug Metabolism and PK/PD Study, Institute of Materia Medica, Chinese Academy of Medical Sciences and Peking Union Medical College, Beijing, 100050, China.

Angewandte Chemie (International ed. in English)

|June 16, 2023

概括

研究人员描述了CsCTS,这是来自Cephalotaxus sinensis的一种新型二二烯合成酶. 这种酶启动了塞法洛坦类型的二聚胺生物合成,揭示了它对复杂自然产品的独特循环化机制.

科学领域:

自然产品生物合成自然产品生物合成
酶学是一种酶学.
有机化学有机化学

背景情况:

塞法洛坦类型的二烯酸是复杂的自然产品,具有刚性四环骨架.
它们的生物合成涉及复杂的循环化步骤,由二合成酶催化.
了解这些酶对于天然产品合成和药物发现至关重要.

研究的目的:

为了功能性地表征CsCTS,来自Cephalotaxus sinensis的一种新型二烯合成酶.
为了阐明头皮素形成的逐步循环化机制.
为了确定参与催化过程的关键氨基酸残留物.

主要方法:

CsCTS的功能性特征.
脱轨产品的结构调查.
同位素标记实验和密度函数理论 (DFT) 计算.
同性学建模,分子动力学 (MD) 模拟和位点定向突变发生.

主要成果:

CsCTS催化了头二烯的形成,这是头二烯类型二二烯的核心骨架.
提出并验证了一种逐步的碳酸驱动级联循环机制.
确定了控制独特循环化的关键氨基酸残留物.

结论:

发现和表征CsCTS,该酶负责首次承诺步骤的头叶类型二二化物生物合成.
独特的循环化机制的划定为我们提供了关于特特类自然产物形成的见解.
这项工作为破译和设计完整的生物合成途径奠定了基础.

关键词:

塞法洛坦类型的迪特尔类.塞法洛塔克萨斯 (Cephalotaxus Sinensis) 是一个大脑.迪特尔合成酶的使用方法酶的机制酶的机制同位素标签的标记

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