Three Redundant Synthetases Secure Redox-Active Pigment Production in the Basidiomycete Paxillus involutus

Three Redundant Synthetases Secure Redox-Active Pigment Production in the Basidiomycete Paxillus involutus
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DOI:
10.1016/j.chembiol.2015.08.016
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发表时间:
2015-10-22
影响因子:
--
通讯作者:
Hoffmeister, Dirk
Hoffmeister, Dirk
中科院分区:
生物1区
文献类型:
--
作者:
Braesel, Jana;Goetze, Sebastian;Hoffmeister, Dirk

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这种共生真菌在维持森林生态系统方面起着至关重要的作用,森林生态系统是具有全球重要性的碳汇。不合拟青霉产生内含素和其他2,5-二芳基环戊酮色素,这些色素可能通过芬顿化学帮助木质纤维素的氧化降解。然而,它们的确切生物合成途径仍然不清楚。利用生化、遗传和转录分析的组合,除了用合成前体进行稳定同位素标记外,我们还表明阿托明是关键的中间体。Atroentin是由高度相似的三域合成酶:InvA1、InvA2和InvA5合成的。失活的萎缩素合成酶InvA3在结构域交换后获得了活性,该结构域用InvA5取代了其天然的硫酯酶结构域。对于真菌来说,多重生物合成能力的发现程度是史无前例的,这突显了代谢物对生产者的重要性。
The symbiotic fungus Paxillus involutus serves a critical role in maintaining forest ecosystems, which are carbon sinks of global importance. P. involutus produces involutin and other 2,5-diarylcyclopentenone pigments that presumably assist in the oxidative degradation of lignocellulose via Fenton chemistry. Their precise biosynthetic pathways, however, remain obscure. Using a combination of biochemical, genetic, and transcriptomic analyses, in addition to stable-isotope labeling with synthetic precursors, we show that atromentin is the key intermediate. Atromentin is made by tridomain synthetases of high similarity: InvA1, InvA2, and InvA5. An inactive atromentin synthetase, InvA3, gained activity after a domain swap that replaced its native thioesterase domain with that of InvA5. The found degree of multiplex biosynthetic capacity is unprecedented with fungi, and highlights the great importance of the metabolite for the producer.