Novel Methoxymethacrylate Natural Products Uncovered by Statistics-Based Mining of the Myxococcus fulvus Secondary Metabolome.,ACS Chemical Biology

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Novel Methoxymethacrylate Natural Products Uncovered by Statistics-Based Mining of the Myxococcus fulvus Secondary Metabolome.
ACS Chemical Biology ( IF 3.5 ) Pub Date : 2019-01-02 , DOI: 10.1021/acschembio.8b00948
Fabian Panter _{1,

2} , Daniel Krug _{1,

2} , Rolf Müller _{1,

2}

Affiliation

This study reports the uncovering of new myxobacterial natural products through comprehensive analysis of the Myxococcus fulvus secondary metabolome. Statistics-based mining of mass spectrometry data paved the way for full structure elucidation of two new secondary metabolites named fulvuthiacene A and B, and investigation of the underlying biosynthetic pathway revealed an evolutionary link between the fulvuthiacene hybrid polyketide synthase (PKS) and nonribosomal peptide synthetase (NRPS) gene cluster and the related myxothiazol and melithiazol assembly lines. Detailed characterization of the post-PKS modification enzyme cascade responsible for the fulvuthiacenes' terminal β-methoxy-methyl acrylate moiety was pursued by heterologous expression of these enzymes in the myxothiazol producer Stigmatella aurantiaca DW4/3-1. The discovery of fulvuthiacenes provides new insights into the overall structure-activity relationship picture for the β-methoxyacrylate class of respiratory chain inhibitors and might thus serve as starting point for the development of next-generation β-methoxymethacrylate fungicides.

中文翻译：

通过基于统计的黄霉菌次生代谢组的挖掘发现的新型甲氧基甲基丙烯酸甲酯天然产物。

这项研究报告了通过对黄粉球菌次生代谢组的综合分析发现了新的粘菌天然产物。基于统计数据的质谱数据挖掘为两种新的二级代谢物富伏特噻辛烯A和B的全结构阐明铺平了道路，对基础生物合成途径的研究揭示了富伏特硫辛烯混合聚酮化合物合酶（PKS）和非核糖体肽合成酶之间的进化联系（NRPS）基因簇以及相关的甲噻唑和甲石唑组装线。通过在甲氧噻唑生产商autigica aurantiaca DW4 / 3-1中异源表达这些酶来追踪负责全氟噻菌胺末端β-甲氧基-甲基丙烯酸酯部分的PKS后修饰酶级联反应的详细特征。

更新日期：2018-12-13

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