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Gas-phase NO+ affinities

F Cacace1, G de Petris, F Pepi

  • 1Dipartimento di Studi di Chimica e Tecnologia delle Sostanze Biologicamente Attive, Università degli Studi di Roma La Sapienza, Rome, Italy.

Proceedings of the National Academy of Sciences of the United States of America
|April 15, 1997
PubMed
Summary

This study establishes a gas-phase NO+ binding energy scale for 52 ligands using mass spectrometry. The findings reveal a linear correlation between NO+ binding energies and proton affinities, enabling accurate predictions for various molecules.

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Area of Science:

  • Physical Chemistry
  • Chemical Thermodynamics
  • Mass Spectrometry

Background:

  • Accurate determination of gas-phase binding energies (BEs) is crucial for understanding molecular interactions.
  • Previous studies on NO+ binding energies have shown discrepancies, necessitating a refined scale.
  • The kinetic method and NO+-transfer equilibria are established techniques for gas-phase ion studies.

Purpose of the Study:

  • To construct a comprehensive relative and absolute gas-phase NO+ binding energy scale for a diverse set of 52 ligands.
  • To investigate the relationship between NO+ binding energies and proton affinities (PAs).
  • To extend the applicability of the kinetic method for evaluating absolute binding energies of polyatomic cations.

Main Methods:

  • Utilized Fourier-transform ion cyclotron resonance mass spectrometry to evaluate NO+-transfer equilibria.

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  • Employed the kinetic method based on metastable fragmentation of nitryl-ion bound dimers.
  • Established a relative scale anchored to the NO+ affinity of water, leading to an absolute scale.

    • Main Results:

    • A relative gas-phase NO+ binding energy scale for 52 ligands was constructed, including alkyl halides, nitrates, alcohols, and aromatic compounds.
    • A linear correlation was observed between NO+ binding energies and proton affinities, with NO+ BEs being lower than PAs but higher than NO2+ BEs.
    • The established correlation allows for the prediction of NO+ binding energies for molecules in existing PA compilations, with high accuracy (1-2 kcal x mol(-1)).

    Conclusions:

    • The study successfully established a reliable gas-phase NO+ binding energy scale and demonstrated its utility in predicting binding energies.
    • The linear correlation between NO+ BEs and PAs provides a valuable tool for computational and experimental chemists.
    • The findings are consistent with existing theoretical and experimental data on the stability of NO+ and NO2+ complexes.