Chemoenzymatic elaboration of the Raper–Mason pathway unravels the structural diversity within eumelanin pigments,Chemical Science

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Chemoenzymatic elaboration of the Raper–Mason pathway unravels the structural diversity within eumelanin pigments
Chemical Science ( IF 7.6 ) Pub Date : 2020-07-09 , DOI: 10.1039/d0sc02262d
Qing Zhe Ni _{1,

2,

3,

4} , Brianna N. Sierra _{1,

2,

3,

4} , James J. La Clair _{1,

2,

3,

4} , Michael D. Burkart _{1,

2,

3,

4}

Affiliation

Melanin is a central polymer in living organisms, yet our understanding of its molecular structure remains unresolved. Here, we apply a biosynthetic approach to explore the composite structures accessible in one type of melanin, eumelanin. Using a combination of solid-state NMR, dynamic nuclear polarization, and electron microscopy, we reveal how a variety of monomers are enzymatically polymerized into their corresponding eumelanin pigments. We demonstrate how this approach can be used to unite structure with an understanding of enzymatic activity, substrate scope, and the regulation of nanostructural features. Overall, this data reveals how intermediate metabolites of the Raper–Mason metabolic pathway contribute to polymerization, allowing us to revisit the original proposal of how eumelanin is biosynthesized.

中文翻译：

Raper-Mason途径的化学酶解揭示了真木兰色素内的结构多样性

黑色素是生物体中的核心聚合物，但我们对其分子结构的理解仍未解决。在这里，我们应用一种生物合成方法来探索一种黑色素-Eumelanin中可访问的复合结构。结合使用固态NMR，动态核极化和电子显微镜，我们揭示了各种单体如何酶促聚合成其相应的Eumelanin颜料。我们展示了如何使用这种方法结合酶活性，底物范围和纳米结构特征的调控来统一结构。总体而言，这些数据揭示了Raper-Mason代谢途径的中间代谢物如何促进聚合，从而使我们能够重新审视关于如何合成双美金的最初建议。

更新日期：2020-08-05

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