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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Hydroxymalonyl-acyl carrier protein (ACP) and aminomalonyl-ACP are two additional type Ⅰ polyketide synthase extender units
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Hydroxymalonyl-acyl carrier protein (ACP) and aminomalonyl-ACP are two additional type Ⅰ polyketide synthase extender units

机译：羟丙二酸-酰基载体蛋白（ACP）和氨基丙二酸-ACP是另外两个Ⅰ型聚酮化合物合酶扩展剂单元

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摘要

Combinatorial biosynthesis of type Ⅰ polyketide synthases is a promising approach for the generation of new structural derivatives of polyketide-containing natural products. A target of this approach has been to change the extender units incorporated into a polyketide backbone to alter the structure and activity of the natural product. One limitation to these efforts is that only four extender units were known: malonyl-CoA, methylmalonyl-CoA, ethylmalonyl-CoA, and methoxymalonyl-acyl carrier protein (ACP). The chemical attributes of these extender units are quite similar, with the exception of the potential hydrogen bonding interactions by the oxygen of the methoxy moiety. Furthermore, the incorporated extender units are not easily modified by using simple chemical approaches when combinatorial biosynthesis is coupled to semisynthetic chemistry. We recently proposed the existence of two additional extender units, hydroxymalonyl-ACP and aminomalonyl-ACP, involved in the biosynthesis of zwittermicin A. These extender units offer unique possibilities for combinatorial biosynthesis and semisynthetic chemistry because of the introduction of free hydroxyl and amino moieties into a polyketide structure. Here, we present the biochemical and mass spectral evidence for the formation of these extender units. This evidence shows the formation of ACP-linked extender units for polyketide synthesis. Interestingly, aminomalonyl-ACP formation involves enzymology typically found in nonribosomal peptide synthesis.
机译：Ⅰ型聚酮化合物合酶的组合生物合成是一种产生含聚酮化合物天然产物的新结构衍生物的有前途的方法。该方法的目标是改变掺入聚酮骨架中的增量剂单元，以改变天然产物的结构和活性。这些努力的局限性是仅已知四个增量剂单元：丙二酰辅酶A，甲基丙二酰辅酶A，乙基丙二酰辅酶A和甲氧基丙二酰酰基载体蛋白（ACP）。除了由甲氧基部分的氧引起的潜在氢键相互作用以外，这些增量剂单元的化学性质非常相似。此外，当组合生物合成与半合成化学偶联时，通过使用简单的化学方法不容易修饰引入的增量剂单元。我们最近提出了存在另外两个增量剂单元，即羟基异戊二烯-ACP和氨基丙二酸-ACP，它们参与了两维特霉素A的生物合成。由于将游离的羟基和氨基引入到生物合成和半合成化学中，这些扩展剂提供了独特的可能性。聚酮化合物结构。在这里，我们介绍了这些扩展单元的形成的生化和质谱证据。该证据显示了用于聚酮化合物合成的ACP连接的扩展单元的形成。有趣的是，氨基丙二酰基-ACP的形成涉及通常在非核糖体肽合成中发现的酶学。

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