Isolation and structure determination of diazonamides A and B, unusual cytotoxic metabolites from the marine ascidian Diazona chinensis

Journal of the American Chemical Society
1991.0

Abstract

We investigated the secondary metabolites of the colonial ascidian Diazona chinensis collected from the northwest coast of Siquijor Island, Philippines. We report the structures of diazonamides A (1) and B (2), two unusual halogenated cyclic peptides with potent in vitro cytotoxic activity. The combined organic extract of the lyophilized ascidian was partitioned between hexane and methanol, and the methanol-soluble material was further partitioned between butanol and water. Gel filtration of the butanol-soluble material on Sephadex LH-20 with methanol followed by reverse-phase HPLC (ODS-silica) using 9:1 methanol/water gave pure diazonamides A (1, 54 mg, 0.021% dry weight) and B (2, 132 mg, 0.052%). Their structures were established by a combination of ¹H NMR, ¹³C NMR, and HRFABMS experiments, and single-crystal X-ray diffraction analysis of the p-bromobenzamide derivative of diazonamide B (3). Diazonamides A and B represent an entirely new class of halogenated, highly unsaturated cyclic peptides containing derivatives of at least three common amino acids: a 3,4,5-trisubstituted L-tyrosine (C1-C9), a tryptophan substituted at the 2- and 4-positions of the indole (C18-C27), and an L-valine (C31-C35), forming an extremely rigid framework with essentially no conformational freedom for the polycyclic core. Diazonamide A has potent in vitro activity against HCT-116 human colon carcinoma and B-16 murine melanoma cancer cell lines, with IC₅₀ values less than 15 ng/mL, while diazonamide B is less active.

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