Immunosuppressive Polyketides from Mantis-Associated Daldinia eschscholzii

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• 作者：Ying L. Zhang ; Jie Zhang ; Nan Jiang ; Yan H. Lu ; Lu Wang ; Su H. Xu ; Wei Wang ; Gao F. Zhang ; Qiang Xu ; Hui M. Ge ; Jing Ma ; Yong C. Song ; Ren X. Tan
• 刊名：Journal of the American Chemical Society
• 出版年：2011
• 出版时间：April 20, 2011
• 年：2011
• 卷：133
• 期：15
• 页码：5931-5940
• 全文大小：1151K
• 年卷期：v.133,no.15(April 20, 2011)
• ISSN：1520-5126

文摘

Polyketides with unknown architectures are highly desired for the discovery of new drugs and agrochemicals. Here, the mantis-associated Daldinia eschscholzii, a fungus known to produce immunosuppressants dalesconols A and B, was found to simultaneously generate four novel skeletons capable of shaping the unusual chemistry of the fungal polyketides, of which seven were structurally unique and substantially immunosuppressive. In particular, the scaled-up fermentation of the microbe enabled the structural characterization of minor or 鈥渢ransitional鈥?intermediate polyketides that allowed the reasonable recognition of the four biosynthetic pathways initiated by condensations of four, five, six and eight acetate units, respectively. Furthermore, the decarbonylation reaction of triketone, as in the case of daeschol A, was described for the first time, in addition to the structural correction of sporothrin C and nodulone. The work provided a set of novel immunosuppressive molecules that are of significance to drug discovery.