Synthesis of the 16S,17S-Epoxyprotectin Intermediate in the Biosynthesis of Protectins by Human Macrophages

J Nat Prod. 2015 Dec 24;78(12):2924-31. doi: 10.1021/acs.jnatprod.5b00574. Epub 2015 Nov 18.

Abstract

The n-3 polyunsaturated fatty acids act as substrates during the resolution phase of acute inflammation for the biosynthesis of specialized pro-resolving lipid mediators. One premier example is the C22-dihydroxy-polyunsaturated fatty acid protectin D1 (1). The human 15-lipoxygenase type I, via stereoselective processes and with docosahexaenoic acid as the substrate, enables the formation of this specialized pro-resolving lipid mediator. Herein, based on results from LC/MS-MS metabololipidomics, support is presented for the apprehended biosynthesis of 1 in human macrophages occurring via the intermediate 16S,17S-epoxyprotectin (5). Stereochemically pure 5 was obtained using the Katsuki-Sharpless epoxidation protocol, establishing the chirality at the C16 and C17 atoms, one Z-selective reduction, and E- and Z-stereoselective Wittig reactions. In addition, information on the nonenzymatic aqueous hydrolysis products and the half-life of 16S,17S-epoxyprotectin (5) is presented.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • CD59 Antigens
  • Catalysis
  • Chromatography, Liquid
  • Docosahexaenoic Acids / biosynthesis*
  • Docosahexaenoic Acids / chemistry
  • Fatty Acids, Unsaturated / metabolism
  • Humans
  • Inflammation / metabolism
  • Macrophages / metabolism*
  • Molecular Structure
  • Stereoisomerism

Substances

  • 16S,17S-epoxyprotectin
  • CD59 Antigens
  • Fatty Acids, Unsaturated
  • protectin D1
  • Docosahexaenoic Acids