Debromomarinone Explained

Debromomarinone is a chemical compound isolated from marine actinomycetes.[1]

Biosynthesis

The proposed biosynthesis of marinone was first reported by Murray et al. in 2018.[2] The biosynthesis of marinone begins with 1,3,6,8-tetrahydroxynaphthalene (THN), which is known to be biosynthesized via the condensation of five malonyl-coenzyme A units followed by the aromatization of the resulting pentaketide using a type III polyketide synthase.[3] Next, THN undergoes geranylation or farnesylation at the C-4 position, yielding 1 (Fig. 1). This transformation is catalyzed in vivo by NphB aromatic prenyltransferase in naphterpin biosynthesis[4] or by CnqP3 or CnqP4 in marinone biosynthesis.[5] Then, 1 undergoes oxidative dearomatization which is catalyzed by VCPO, which is a vanadium-dependent chloroperoxidase enzyme. This transformation yields compound 2. Compound 2 then undergoes two consecutive chlorinations at the C2 position, catalyzed by VCPO, to yield 4. Next, a VCPO catalyzed α-hydroxyketone rearrangement shifts the geranyl substituent from C-4 to C-3, yielding 5. Exposure of 5 to mildly basic conditions induces cyclization to yield the α-chloroepoxide, 6. This is followed by the reductive halogenation of the α-chloroepoxide to yield the hydroxynaphthoquinone, 7. Next, oxidation at the C-2 position and facile E/Z isomerization of the double bond affords the enone, 8, which undergoes a intramolecular hetero-Diels-Alder to yield debromomarinone.

Notes and References

  1. 7710421 . 1995 . Mikhaĭlov . V. V. . Bioactive compounds from marine actinomycetes . Bioorganicheskaia Khimiia . 21 . 1 . 3–8 . Kuznetsova . T. A. . Eliakov . G. B. .
  2. Murray LA, McKinnie SM, Pepper HP, Erni R, Miles ZD, Cruickshank MC, López-Pérez B, Moore BS, George JH . 6 . Total Synthesis Establishes the Biosynthetic Pathway to the Naphterpin and Marinone Natural Products . Angewandte Chemie . 57 . 34 . 11009–11014 . August 2018 . 29935040 . 10.1002/anie.201804351 . 6248334 .
  3. Shen X, Wang X, Huang T, Deng Z, Lin S . Naphthoquinone-Based Meroterpenoids from Marine-Derived Streptomyces sp. B9173 . Biomolecules . 10 . 8 . 1187 . August 2020 . 32824158 . 7463872 . 10.3390/biom10081187 . free .
  4. Kuzuyama T, Noel JP, Richard SB . Structural basis for the promiscuous biosynthetic prenylation of aromatic natural products . Nature . 435 . 7044 . 983–987 . June 2005 . 15959519 . 2874460 . 10.1038/nature03668 . 2005Natur.435..983K .
  5. Motohashi K, Irie K, Toda T, Matsuo Y, Kasai H, Sue M, Furihata K, Seto H . 6 . Studies on terpenoids produced by actinomycetes. 5-dimethylallylindole-3-carboxylic Acid and A80915G-8"-acid produced by marine-derived Streptomyces sp. MS239 . The Journal of Antibiotics . 61 . 2 . 75–80 . February 2008 . 18408326 . 10.1038/ja.2008.113 . 29628302 . free .