Radical S-Adenosylmethionine Enzymes Involved in RiPP Biosynthesis.
Radical S-Adenosylmethionine Enzymes Involved in RiPP Biosynthesis.
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DOI：
10.1021/acs.biochem.7b00771
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发表时间：
2017-10-10
期刊：
影响因子：
2.9
通讯作者：
Mitchell DA
中科院分区：
文献类型：
--
作者：
Mahanta N;Hudson GA;Mitchell DA
核糖体合成和翻译后修饰肽 (RiPP) 显示出多种结构，并作为天然产品类别不断扩展。因此，RiPP 表现出广泛的生物活性，例如广谱和窄谱生长抑制剂、抗糖尿病药、以及镇痛药和抗癌药。由于这些特性以及产生这些分子的复杂翻译后修饰 (PTM)，RiPP 生物合成已得到深入研究。 RiPP 生物合成通常涉及具有独特化学反应和有趣反应机制的酶，这吸引了化学家和生物化学家研究和重新设计这些途径。 RiPP 生物合成酶的一种特殊类型是所谓的自由基 S-腺苷甲硫氨酸 (rSAM) 酶，它利用基于自由基的化学来安装几种不同的 PTM。在这里，我们描述了过去十年中表征的 rSAM 酶，这些酶催化来自多种 RiPP 生物合成途径的六种反应类型。我们介绍了机制理解的当前状态，并总结了该酶家族未来表征的可能方向。
Ribosomally synthesized and post-translationally modified peptides (RiPPs) display a diverse range of structures and continue to expand as a natural product class. Accordingly, RiPPs exhibit a wide array of bioactivities, such as broad and narrow spectrum growth suppressors, antidiabetics, as well as antinociception and anticancer agents. Owing to these properties, and the complex repertoire of post-translational modifications (PTMs) that give rise to these molecules, RiPP biosynthesis has been intensely studied. RiPP biosynthesis often involves enzymes that perform unique chemistry with intriguing reaction mechanisms, which attract chemists and biochemists alike to study and re-engineer these pathways. One particular type of RiPP biosynthetic enzyme is the so-called radical S-adenosylmethionine (rSAM) enzyme, which utilize radical-based chemistry to install several distinct PTMs. Here, we describe the rSAM enzymes characterized over the past decade that catalyze six reactions types from several RiPP biosynthetic pathways. We present the current state of mechanistic understanding and conclude with possible directions for future characterization of this enzyme family.
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