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From a Natural Product to Its Biosynthetic Gene Cluster: A Demonstration Using Polyketomycin from Streptomyces diastatochromogenes Tü6028
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Freedom and constraint in engineered noncolinear polyketide assembly lines
Yuki Sugimoto1, Keishi Ishida1, Nelly Traitcheva1
1Department of Biomolecular Chemistry, Leibniz Institute for Natural Product Research and Infection Biology (HKI), Beutenbergstr. 11a, 07745 Jena, Germany.
Chemistry & Biology
|February 10, 2015
Summary
Polyketide synthases (PKS) can iteratively assemble complex molecules. This study reveals the adaptability of iterative PKS modules and their role in controlling polyketide chain length, offering insights into natural product biosynthesis.
Area of Science:
- Biochemistry
- Molecular Biology
- Natural Product Synthesis
Background:
- Modular type I polyketide synthases (PKS) are crucial for synthesizing pharmacologically important natural products.
- Most PKS enzymes function unidirectionally, but exceptions exist for producing nitro-substituted polyketides like neoaureothin and aureothin.
Purpose of the Study:
- Investigate the flexibility of the neoaureothin (nor) PKS.
- Identify factors influencing iterative elongation by noncanonical modules.
- Explore the potential of truncated nor PKS variants in artificial assembly lines.
Main Methods:
- Enzymatic assays using truncated nor PKS variants.
- Construction of artificial assembly lines for aureothin and homoaureothin synthesis.
- Analysis of polypropionate derivatives to understand chain length control.
Main Results:
- The nor PKS demonstrated plasticity, enabling an additional chain elongation to produce homoneoaureothin.
- Truncated nor PKS variants were successfully used in artificial assembly lines.
- Synthesized polypropionate derivatives revealed structure-activity relationships based on backbone size.
Conclusions:
- Iterative PKS modules exhibit significant adaptability in natural product biosynthesis.
- Downstream PKS modules act as gatekeepers, ensuring the selection of correctly sized polyketide chains.
- Findings provide insights into polyketide chain length determination and PKS engineering.
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