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Gas-phase nitronium ion affinities.

F Cacace1, G de Petris, F Pepi

  • 1Dipartimento di Studi di Chimica e Tecnologia della Sustanze Biologicamente Attive, Università degli Studi di Roma "La Sapienza," Rome, Italy.

Proceedings of the National Academy of Sciences of the United States of America
|September 12, 1995
PubMed
Summary

Researchers quantified nitronium ion affinities for 18 ligands using mass spectrometry. They found a correlation between nitronium ion affinities and proton affinities, useful for predicting molecular properties.

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Area of Science:

  • Physical Chemistry
  • Gas-Phase Ion Chemistry
  • Mass Spectrometry

Background:

  • Nitronium ion (NO2+) affinities are crucial for understanding chemical reactivity and molecular interactions.
  • Previous studies have lacked a comprehensive scale for NO2+ affinities across diverse ligands.
  • The kinetic method and ion-transfer equilibria provide avenues for thermodynamic measurements.

Purpose of the Study:

  • To establish a relative and absolute gas-phase nitronium ion affinity scale for various ligands.
  • To investigate the correlation between nitronium ion affinities and proton affinities.
  • To extend the kinetic method to polyatomic ion-bound dimers.

Main Methods:

  • Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was employed to measure ion-transfer equilibria.

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  • The kinetic method, analyzing metastable fragmentation of nitronium ion-bound dimers, was applied.
  • The established affinity scale was calibrated using a literature value for water's NO2+ affinity.

    • Main Results:

    • A scale of relative and absolute gas-phase NO2+ affinities was determined for 18 ligands.
    • A reasonably linear correlation was observed between NO2+ affinities and proton affinities (PAs) for diverse ligands.
    • NO2+ binding energies were found to be significantly lower than PAs and related cation binding energies.

    Conclusions:

    • The study provides a valuable tool for predicting NO2+ affinities based on PAs, with improved linearity for specific ligand classes.
    • The extension of the kinetic method broadens its applicability to polyatomic ions.
    • Experimental determination of ammonia's NO2+ affinity enabled the evaluation of nitramide's amino group PA, verifying theoretical predictions.