Fluoroacetamide Moieties as NMR Spectroscopy Probes for the Molecular Recognition of GlcNAc-Containing Sugars: Modulation of the CH-π Stacking Interactions by Different Fluorination Patterns

Chemistry. 2017 Mar 17;23(16):3957-3965. doi: 10.1002/chem.201605573. Epub 2017 Feb 23.

Abstract

We herein propose the use of fluoroacetamide and difluoroacetamide moieties as sensitive tags for the detection of sugar-protein interactions by simple 1 H and/or 19 F NMR spectroscopy methods. In this process, we have chosen the binding of N,N'-diacetyl chitobiose, a ubiquitous disaccharide fragment in glycoproteins, by wheat-germ agglutinin (WGA), a model lectin. By using saturation-transfer difference (STD)-NMR spectroscopy, we experimentally demonstrate that, under solution conditions, the molecule that contained the CHF2 CONH- moiety is the stronger aromatic binder, followed by the analogue with the CH2 FCONH- group and the natural molecule (with the CH3 CONH- fragment). In contrast, the molecule with the CF3 CONH- isoster displayed the weakest intermolecular interaction (one order of magnitude weaker). Because sugar-aromatic CH-π interactions are at the origin of these observations, these results further contribute to the characterization and exploration of these forces and offer an opportunity to use them to unravel complex recognition processes.

Keywords: NMR spectroscopy; fluorine; molecular modeling; molecular recognition; noncovalent interactions.

MeSH terms

  • Disaccharides / analysis
  • Disaccharides / metabolism*
  • Fluoroacetates / analysis
  • Fluoroacetates / metabolism*
  • Halogenation
  • Magnetic Resonance Spectroscopy / methods*
  • Microarray Analysis
  • Protein Binding
  • Triticum / chemistry
  • Triticum / metabolism
  • Wheat Germ Agglutinins / analysis
  • Wheat Germ Agglutinins / metabolism*

Substances

  • Disaccharides
  • Fluoroacetates
  • Wheat Germ Agglutinins
  • N,N-diacetylchitobiose
  • fluoroacetamide