Clickable analogue of cerulenin as chemical probe to explore protein palmitoylation

ACS Chem Biol. 2015 Jan 16;10(1):115-21. doi: 10.1021/cb500758s. Epub 2014 Oct 23.

Abstract

Dynamic palmitoylation is an important post-translational modification regulating protein localization, trafficking, and signaling activities. The Asp-His-His-Cys (DHHC) domain containing enzymes are evolutionarily conserved palmitoyl acyltransferases (PATs) mediating diverse protein S-palmitoylation. Cerulenin is a natural product inhibitor of fatty acid biosynthesis and protein palmitoylation, through irreversible alkylation of the cysteine residues in the enzymes. Here, we report the synthesis and characterization of a "clickable" and long alkyl chain analogue of cerulenin as a chemical probe to investigate its cellular targets and to label and profile PATs in vitro and in live cells. Our results showed that the probe could stably label the DHHC-family PATs and enable mass spectrometry studies of PATs and other target proteins in the cellular proteome. Such probe provides a new chemical tool to dissect the functions of palmitoylating enzymes in cell signaling and diseases and reveals new cellular targets of the natural product cerulenin.

Publication types

  • Letter
  • Research Support, Non-U.S. Gov't

MeSH terms

  • 1-Acylglycerophosphocholine O-Acyltransferase / chemistry
  • 1-Acylglycerophosphocholine O-Acyltransferase / metabolism
  • Acyltransferases / chemistry
  • Acyltransferases / metabolism
  • Animals
  • Cerulenin* / analogs & derivatives
  • Cerulenin* / chemical synthesis
  • Click Chemistry
  • Humans
  • Lipoylation*
  • Molecular Probes* / chemical synthesis
  • Molecular Probes* / chemistry
  • Protein Processing, Post-Translational*
  • Proteins / chemistry
  • Proteins / metabolism*
  • Thiolester Hydrolases / chemistry
  • Thiolester Hydrolases / metabolism

Substances

  • Molecular Probes
  • Proteins
  • Cerulenin
  • Acyltransferases
  • 1-Acylglycerophosphocholine O-Acyltransferase
  • LPCAT2 protein, human
  • LYPLA1 protein, human
  • Thiolester Hydrolases