ArticleACS chemical biology2019
Evolutionary Trajectories for the Functional Diversification of Anthracycline Methyltransferases.
Article in ACS chemical biology, 2019. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 7 papers.
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Who cites it
7 citing papers in PubMed, 16 citations in OpenAlex.
- PhyloNaP: a user-friendly database of phylogeny for natural product-producing enzymes.Bioinformatics (Oxford, England) · 2026Article
- Diverse Combinatorial Biosynthesis Strategies for C-H Functionalization of Anthracyclinones.ACS synthetic biology · 2024Article
- Biochemical and Structural Studies of the Carminomycin 4-Journal of natural products · 2024Article
- Evolution-inspired engineering of anthracycline methyltransferases.PNAS nexus · 2023Article
- A BioBricks Metabolic Engineering Platform for the Biosynthesis of Anthracyclinones inACS synthetic biology · 2022Article
- Activation and discovery of tsukubarubicin from Streptomyces tsukubaensis through overexpressing SARPs.Applied microbiology and biotechnology · 2021Article
- Synthetic biology enabling access to designer polyketides.Current opinion in chemical biology · 2020Review
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Authors and funding
6 authors at 1 institution in 1 country.
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Abstract
Microbial natural products are an important source of chemical entities for drug discovery. Recent advances in understanding the biosynthesis of secondary metabolites has revealed how this rich chemical diversity is generated through functional differentiation of biosynthetic enzymes. For instance, investigations into anthracycline anticancer agents have uncovered distinct S-adenosyl methionine (SAM)-dependent proteins: DnrK is a 4-O-methyltransferase involved in daunorubicin biosynthesis, whereas RdmB (52% sequence identity) from the rhodomycin pathway catalyzes 10-hydroxylation. Here, we have mined unknown anthracycline gene clusters and discovered a third protein subclass catalyzing 10-decarboxylation. Subsequent isolation of komodoquinone B from two Streptomyces strains verified the biological relevance of the decarboxylation activity. Phylogenetic analysis inferred two independent routes for the conversion of methyltransferases into hydroxylases, with a two-step process involving loss-of-methylation and gain-of-hydroxylation presented here. Finally, we show that simultaneously with the functional differentiation, the evolutionary process has led to alterations in substrate specificities.
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