Fluorinated aromatic amino acids are sensitive 19F NMR probes for bromodomain-ligand interactions

ACS Chem Biol. 2014 Dec 19;9(12):2755-60. doi: 10.1021/cb5007344. Epub 2014 Oct 27.

Abstract

We describe a (19)F NMR method for detecting bromodomain-ligand interactions using fluorine-labeled aromatic amino acids due to the conservation of aromatic residues in the bromodomain binding site. We test the sensitivity, accuracy, and speed of this method with small molecule ligands (+)-JQ1, BI2536, Dinaciclib, TG101348, and acetaminophen using three bromodomains Brd4, BrdT, and BPTF. Simplified (19)F NMR spectra allowed for simultaneous testing of multiple bromodomains to assess selectivity and identification of a new BPTF ligand. Fluorine labeling only modestly affected the Brd4 structure and function assessed by isothermal titration calorimetry, circular dichroism, and X-ray crystallography. The speed, ease of interpretation, and low concentration of protein needed for binding experiments affords a new method to discover and characterize both native and new ligands.

Publication types

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

MeSH terms

  • Acetaminophen / chemistry
  • Amino Acids, Aromatic / chemistry*
  • Antigens, Nuclear / chemistry
  • Antigens, Nuclear / genetics
  • Azepines / chemistry
  • Binding Sites
  • Bridged Bicyclo Compounds, Heterocyclic / chemistry
  • Cell Cycle Proteins
  • Crystallography, X-Ray
  • Cyclic N-Oxides
  • Escherichia coli / genetics
  • Escherichia coli / metabolism
  • Gene Expression
  • Halogenation
  • Humans
  • Indolizines
  • Ligands
  • Magnetic Resonance Spectroscopy / methods
  • Molecular Docking Simulation
  • Molecular Probes / chemistry*
  • Nerve Tissue Proteins / chemistry
  • Nerve Tissue Proteins / genetics
  • Nuclear Proteins / chemistry
  • Nuclear Proteins / genetics
  • Oncogene Proteins, Fusion / chemistry*
  • Oncogene Proteins, Fusion / genetics
  • Protein Binding
  • Pteridines / chemistry
  • Pyridinium Compounds / chemistry
  • Pyrrolidines / chemistry
  • Recombinant Proteins / chemistry
  • Recombinant Proteins / genetics
  • Staining and Labeling / methods
  • Sulfonamides / chemistry
  • Transcription Factors / chemistry
  • Transcription Factors / genetics
  • Triazoles / chemistry

Substances

  • (+)-JQ1 compound
  • Amino Acids, Aromatic
  • Antigens, Nuclear
  • Azepines
  • BI 2536
  • BRD4 protein, human
  • BRDT protein, human
  • Bridged Bicyclo Compounds, Heterocyclic
  • Cell Cycle Proteins
  • Cyclic N-Oxides
  • Indolizines
  • Ligands
  • Molecular Probes
  • Nerve Tissue Proteins
  • Nuclear Proteins
  • Oncogene Proteins, Fusion
  • Pteridines
  • Pyridinium Compounds
  • Pyrrolidines
  • Recombinant Proteins
  • Sulfonamides
  • Transcription Factors
  • Triazoles
  • fetal Alzheimer antigen
  • Acetaminophen
  • dinaciclib
  • fedratinib