Department of Biomolecular Chemistry, Leibniz Institute for Natural Product Chemistry and Infection Biology (HKI), Beutenbergstr. 11a, 07745, Jena, Germany.
BioPilotPlant, Leibniz Institute for Natural Product Chemistry and Infection Biology (HKI), Beutenbergstr. 11a, 07745, Jena, Germany.
Chemistry. 2020 Dec 4;26(68):15855-15858. doi: 10.1002/chem.202003500. Epub 2020 Nov 3.
The anaerobe Clostridium acetobutylicum belongs to the most important industrially used bacteria. Whereas genome mining points to a high potential for secondary metabolism in C. acetobutylicum, the functions of most biosynthetic gene clusters are cryptic. We report that the addition of supra-physiological concentrations of cysteine triggered the formation of a novel natural product, clostrisulfone (1). Its structure was fully elucidated by NMR, MS and the chemical synthesis of a reference compound. Clostrisulfone is the first reported natural product with a diphenylsulfone scaffold. A biomimetic synthesis suggests that pentamethylchromanol-derived radicals capture sulfur dioxide to form 1. In a cell-based assay using murine macrophages a biphasic and dose-dependent regulation of the LPS-induced release of nitric oxide was observed in the presence of 1.
产丁酸梭菌(Clostridium acetobutylicum)属于最重要的工业用细菌之一。虽然基因组挖掘表明产丁酸梭菌具有很高的次生代谢潜力,但大多数生物合成基因簇的功能是隐藏的。我们报告说,添加超生理浓度的半胱氨酸会触发一种新型天然产物——clostrisulfone(1)的形成。通过 NMR、MS 和参考化合物的化学合成,完全阐明了其结构。Clostrisulfone 是第一个报道的具有二苯砜支架的天然产物。生物模拟合成表明,来源于五甲基色醇的自由基捕获二氧化硫以形成 1。在使用小鼠巨噬细胞的基于细胞的测定中,在存在 1 的情况下,观察到 LPS 诱导的一氧化氮释放呈双相和剂量依赖性调节。