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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Ectopic expression of the minimal whiE polyketide synthase generates a library of aromatic polyketides of diverse sizes and shapes
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Ectopic expression of the minimal whiE polyketide synthase generates a library of aromatic polyketides of diverse sizes and shapes

机译：最小的whiE聚酮化合物合酶的异位表达可生成各种大小和形状的芳族聚酮化合物库

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摘要

The single recomhinant expressing the Streptomyces coelicolor minimal whiE (spore pigment) polyketide synthase (PKS) is uniquely capable of generating a large array of well more than 30 polyketides, many of which, so far, are novel to this recombinant. The characterized polyketides represent a diverse set of molecules that differ in size (chain length) and shape (cyclization pattern). This combinatorial biosynthetic library is, by far, the largest and most complex of its kind described to date and indicates that the minimal whiE PKS does not independently control polyketide chain length nor dictate the first cyclization event. Rathcr, the minimal PKS enzyme complex must rely on the stabilizing effects of additional subunits (i.e., the cyclase whiE-Offo) to ensure that the chain reaches the full 24 carbons and cyclizes correctly. This dramatic loss of control implies that the growing polyketide chain does not remain enzyme bound, resulting in the spontaneous cyclization of the methyl termi- nus. Among the six characterized dodecaketides, four different first-ring cyclization regiochemistries are represented, including C7/CI2, CS/C13, CIO/C15, and CI3/CIS. The dodecaketide TW93h possesses a unique 2,4- dioxaadamantane ring system and represents a new structural class of polyketides with no related structures isolated from natural or engineered organisms, thus supporting the claim that engineered biosynthesis is capable of producing novel chemotypes.
机译：表达单一链霉菌天蓝色链霉菌最小的whiE（孢子色素）聚酮化合物合酶（PKS）的单一重组子独特地能够产生大量超过30种聚酮化合物，到目前为止，其中许多是该重组子的新发现。表征的聚酮化合物代表了大小（链长）和形状（环化模式）不同的各种分子。迄今为止，该组合生物合成库是迄今为止描述的同类中最大，最复杂的文库，表明最小的PKE PKS不能独立控制聚酮化合物的链长，也不能决定第一个环化事件。最低限度的PKS酶复合物Rathcr必须依赖于其他亚基（即环化酶whiE-Offo）的稳定作用，以确保链达到完整的24个碳原子并正确环化。这种剧烈的失控意味着正在增长的聚酮化合物链不会保持酶结合，导致甲基末端的自发环化。在六个表征的十二聚核苷酸中，代表了四个不同的第一环环化区域化学，包括C7 / CI2，CS / C13，CIO / C15和CI3 / CIS。十二聚醚TW93h具有独特的2,4-二氧杂金刚烷环系统，代表了一种新的聚酮化合物结构类别，没有与天然或工程生物分离的相关结构，因此支持了工程生物合成能够产生新化学型的主张。

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