Author Type

Faculty

Document Type

Article

Abstract

Marine macrolides that selectively disrupt cell cycle events continue to occupy a central position as lead compounds in the ongoing search for novel anticancer agents, [1, 2] highlighted by the recent FDA approval of Halaven (eribulin mesylate, a fully synthetic analogue of the halichondrins) for the treatment of advanced breast cancer.[3] Lithistid sponges have proven to be a particularly fertile source[4] of such biologically relevant polyketide metabolites, including dictyostatin [5] and discodermolide. [5d, 6] As part of a continued program aimed at the discovery of novel bioactive natural products from deepwater marine invertebrates, we have examined the relatively Unexplored [7] lithistid sponge Leiodermatium. A crude extract of Leiodermatium sp. was found to exhibit substantial activity in an assay which identifies antimitotic agents through detection of phosphonucleolin, a marker of mitosis.[8] Bioassay- guided fractionation led to the isolation of leiodermatolide (1, Figure 1), whose unprecedented 16-membered macrolide skeleton, featuring an unsaturated side chain terminating in a d-lactone, has been elucidated through a combination of extensive NMR spectroscopic analysis, comparative DFT GIAO NMR shift calculations, and molecular modeling. Leiodermatolide was found to exhibit potent and selective antimitotic activity (IC50< 10 nm) against a range of human cancer cell lines by inducing G2/M cell cycle arrest, and represents a promising new lead for anticancer drug discovery.

DOI

10.1002/anie.201007719 (doi)

Publication Date

2011

Comments

Florida Atlantic University. Harbor Branch Oceanographic Institute contribution 1825.

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