Unprecedented mechanism of chain length determination in fungal aromatic polyketide synthases.
Unprecedented mechanism of chain length determination in fungal aromatic polyketide synthases.
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DOI：
10.1016/j.chembiol.2004.05.015
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发表时间：
2004-08
影响因子：
--
通讯作者：
A. Watanabe;Y. Ebizuka
中科院分区：
文献类型：
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作者：
A. Watanabe;Y. Ebizuka
真菌芳香族聚酮显示出显着的结构多样性，主要来源于链长和环化模式的变化。它们的基本骨架是由多功能迭代I型聚酮合成酶(PKSS)合成的。最近，我们发现NidulansWa的C-末端硫酯酶(TE)样结构域催化Claisen环化反应形成N-萘吡喃酮YWA1的B-环。在这里，我们报道了由LagenariumColletotrichum lagenariumPKS1的C-末端TE结构域确定链长的前所未有的机制，除了催化Claisen类型的环化外，它还在缩合反应中从酰基载体蛋白结构域截取聚酮亚甲基中间体，产生较短的链长产物。该链长测定系统在包括细菌和植物的PKSS中是一个新的检测系统。TE结构域的功能多样性直接影响芳香族聚酮化合物的结构多样性。LagenariumPKS1.
Fungal aromatic polyketides show remarkable structural diversity fundamentally derived from variations in chain length and cyclization pattern. Their basic skeletons are synthesized by multifunctional iterative type I polyketide synthases (PKSs). Recently, we have found that the C-terminal thioesterase (TE)-like domain ofAspergillus nidulansWA catalyzes Claisen-type cyclization to form the B-ring of naphthopyrone YWA1. Here we report the unprecedented mechanism of chain length determination by the C-terminal TE-like domain ofColletotrichum lagenariumPKS1, which, in addition to catalyzing Claisen-type cyclization, intercepts the polyketomethylene intermediate from the acyl carrier protein domain during the condensation reaction to produce shorter chain length products. This chain length determination system is novel among PKSs, including bacterial and plant PKSs. The functional diversity of the TE-like domain directly influences the structural diversity of aromatic polyketides inC. lagenariumPKS1.