Tetrahedron Letters, Vol. 38, No. 40, pp. 6969-6972, 1997
Pergamon © 1997 Elsevier Science Ltd
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Pitiamide A, a New Chlorinated Lipid from a Mixed Marine Cyanobacterial
Assemblage
Dale G. Nagle ~', Peter U. Park lb, and Valerie J. Paul*
University of Guam Marine Laboratory, U.O.G. Station, Mangilao, Guam 96923, USA
Abstract: Pitiamide A, a new chloro-lipid, was isolated from an extract of a mixed assemblage of
Lyngbya majuscula and a Microcoleus sp. found growing on intact colonies of the hard coral Porites
cylindrica on Guam. The structure was determined by interpretation of 2D-NMR spectra.
© 1997 Elsevier Science Ltd.
Black band disease, a cyanobacterial infection of scleractinian hard corals by Phormidium corallyticum
has been documented to cause coral colony destruction in the western Atlantic and elsewhere.2 Cytotoxic
metabolites, the nakienones A-C and nakitriol, have been isolated from a Synechocystis sp. found overgrowing
(or infecting) an Okinawan species of hard coral) We have recently observed a thin blue-gray tuff-forming
assemblage of Lyngbya majuscula and Microcoleus sp. (approx. 4:1) overgrowing the apical tips of otherwise
healthy, intact branches of the yellow reef-building coral Porites cylindrica at various locations throughout
Micronesia.4
Small cyanobacteria tufts (1-4 cm3) were carefully removed from coral tips and stored at -20* until
extracted with CH2C12/MeOH (I:1). The crude extract strongly deterred feeding by the yellow-banded
parrotfish (Scarus schlegeh), a common reef herbivore found throughout Micronesia: 2D-TLC analysis of the
extracts showed the presence of several UV-active, orange and purple-charring (H2SO 4, heat) relatively non-
polar secondary metabolites. A 752.4 mg portion of the crude extract (1.31 g, dark oil, 28.7 g dry marc) was
fractionated by silica gel column chromatography with a gradient of hexanes to EtOAc to CH2C12 to MeOH.
The fractions eluting with 40% EtOAc/hexanes to 100% EtOAc (v/v) were combined (242.0 mg) and a portion
(210.9 mg) was separated by Sephadex LH-20 chromatography (50% (v/v) CH2C12 in MeOH), and further
purified by repetitive NP-HPLC (75 and 65% EtOAc in hexanes). The two major compounds were
decolorized with activated charcoal. Final purification by NP-HPLC (2% (v/v) MeOH in CH2C12provided
pitiamide A (1, 8.3 rag) and pitiamide B (2, 15.1 mg). 6
Low resolution EIMS examination suggested the presence of a chlorine in the structure of 1 (m/z 381,
8.6% rel. abundance [M] +; 383, 3.1% rel. abundance [M+2]*). Analysis of 1 by t3C NMR and High
resolution ElMS (381.2551; calc. for 381.2434; 70 eV) provided a molecular formula for [M]÷ of
C22H36C1NO 2 (calc. for 5 ° unsaturation). Compound 1 was optically active [trip = -10.3" (C = 3.0, CHC13).
Examination of 1 by IR (neat, x) = 3650-3100, 2959, 2930, 2873, 1709, 1645, 1553 cmt), UV (~ 223 nm,
MeOH), and 'H-NMR data (Table 1) revealed the presence of a ketone, an amide-linkage, a conjugated diene,
and two methyl branches.
Three IH spin systems were assembled by tH-tH COSY (Figure I) and two carbonyl carbons were
confirmed by ~3C-NMR. The ~H-~3CHMBC spectrum facilitated the attachment of spin systems a-c (Figure
1) and the carbonyl moieties. Specifically, 2 and 3-bond couplings from carbonyl carbon C8 (8 214 ppm) to
H29 of partial structure b and H7 and H323 of a allowed for the attachment of a and b through a ketone moiety.
The C14 carbonyl (~ 172.6 ppm) showed 2JcHand 3JcHcouplings to H215 and H216 of c and Hl2a and Hl2b
of b. Attachment of a vinyl chloride to C 1 completed the planar structure of 1. Additionally, a pronounced
6969