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Meta-omic characterization of the marine invertebrate microbial consortium that produces the chemotherapeutic natural product ET-743
Journal article   Open access   Peer reviewed

Meta-omic characterization of the marine invertebrate microbial consortium that produces the chemotherapeutic natural product ET-743

Christopher M Rath, Benjamin Janto, Josh Earl, Azad Ahmed, Fen Z Hu, Luisa Hiller, Meg Dahlgren, Rachael Kreft, Fengan Yu, Jeremy J Wolff, …
ACS chemical biology, v 6(11), pp 1244-1256
18 Nov 2011
PMID: 21875091
url
https://doi.org/10.1021/cb200244tView
Published, Version of Record (VoR) Open

Abstract

E. turbinata natural products metaproteomics metagenomics symbiont tetrahydroisoquinoline Biosynthesis ET-743 Pictet-Spenglerase Yondelis
In many macroorganisms, the ultimate source of potent biologically active natural products has remained elusive due to an inability to identify and culture the producing symbiotic microorganisms. As a model system for developing a meta-omic approach to identify and characterize natural product pathways from invertebrate-derived microbial consortia we chose to investigate the ET-743 (Yondelis®) biosynthetic pathway. This molecule is an approved anti-cancer agent obtained in low abundance (10 −4 –10 −5 % w/w) from the tunicate Ecteinascidia turbinata , and is generated in suitable quantities for clinical use by a lengthy semi-synthetic process. Based on structural similarities to three bacterial secondary metabolites, we hypothesized that ET-743 is the product of a marine bacterial symbiont. Using metagenomic sequencing of total DNA from the tunicate/microbial consortium we targeted and assembled a 35 kb contig containing 25 genes that comprise the core of the NRPS biosynthetic pathway for this valuable anti-cancer agent. Rigorous sequence analysis based on codon usage of two large unlinked contigs suggests that Candidatus Endoecteinascidia frumentensis produces the ET-743 metabolite. Subsequent metaproteomic analysis confirmed expression of three key biosynthetic proteins. Moreover, the predicted activity of an enzyme for assembly of the tetrahydroisoquinoline core of ET-743 was verified in vitro . This work provides a foundation for direct production of the drug and new analogs through metabolic engineering. We expect that the interdisciplinary approach described is applicable to diverse host-symbiont systems that generate valuable natural products for drug discovery and development.

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Collaboration types
Industry collaboration
Domestic collaboration
Web of Science research areas
Biochemistry & Molecular Biology
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