Semisynthetic Derivatives of the Verticillin Class of Natural Products through Acylation of the C11 Hydroxy Group
Document Type
Article
Publication Date
4-8-2021
Department
Physical & Earth Sciences
Abstract
The verticillins, a class of epipolythiodioxopiperazine alkaloids (ETPs) first described 50 years ago with the discovery of verticillin A (1), have gained attention due to their potent activity against cancer cells, noted both in vitro and in vivo. In this study, the complex scaffold afforded through optimized fermentation was used as a feedstock for semisynthetic efforts designed to explore the reactivity of the C11 and C11′ hydroxy substituents. Functionality introduced at these positions would be expected to impact not only the potency but also the pharmacokinetic properties of the resulting compound. With this in mind, verticillin H (2) was used as a starting material to generate nine semisynthetic analogues (4-12) containing a variety of ester, carbonate, carbamate, and sulfonate moieties. Likewise, verticillin A succinate (13) was synthesized from 1 to demonstrate the successful application of this strategy to other ETPs. The synthesized compounds and their corresponding starting materials (i.e., 1 and 2) were screened for activity against a panel of melanoma, breast, and ovarian cancer cell lines: MDA-MB-435, MDA-MB-231, and OVCAR3. All analogues retained IC50 values in the nanomolar range, comparable to, and in some cases more potent than, the parent compounds.
DOI
10.1021/acsmedchemlett.1c00024
First Page
625
Last Page
630
Volume
12
Issue
4
Publication Title
ACS Medicinal Chemistry Letters
Recommended Citation
Amrine, C. S. M, Huntsman, A. C., Doyle, M. G., Burdette, J. E., Pearce, C. J., Fuchs, J. R., and Oberlies, N. H. (2021). Semisynthetic derivatives of the Verticillin class of natural products through acylation of the C11 Hydroxy group. ACS Medicinal Chemistry Letters, 12(4):625-630. doi: 10.1021/acsmedchemlett.1c00024.
Comments
At the time of publication, Chiraz Soumia M. Amrine was affiliated with The University of North Carolina at Greensboro.