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Heteronuclear single-quantum correlation spectroscopy (HSQC) is a 2D NMR technique that reveals one-bond correlations between hydrogen and a heteronucleus. The HSQC experiment is similar to the heteronuclear correlation experiment (HETCOR) but is more sensitive. In the HSQC spectrum, the proton chemical shift is plotted on the horizontal F2 axis, while the 13C chemical shift is plotted on the vertical F1 axis. The corresponding proton and 13C spectra are also shown. The HSQC contour plot does...
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Experimental and theoretical evidence for HS4.

Giulia de Petris1, Antonella Cartoni, Romano Cipollini

  • 1Dipartimento di Chimica e Tecnologie del Farmaco, Università La Sapienza, Piazzale Aldo Moro, 5-00185 Rome, Italy. giulia.depetris@uniromal.it

The Journal of Physical Chemistry. A
|July 4, 2009
PubMed
Summary

Researchers detected the novel radical hydrogen tetrasulfide (HS(4)) in the gas phase. This molecule, featuring an open-chain structure with three sulfur-sulfur bonds, is stable and its conjugate base was also identified.

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Area of Science:

  • Inorganic Chemistry
  • Physical Chemistry
  • Computational Chemistry

Background:

  • Sulfur-hydrogen compounds are crucial in various chemical processes.
  • Understanding the structure and stability of polysulfides is essential for inorganic chemistry.
  • Previous research has explored shorter sulfur-hydrogen chains, but HS(4) remained largely uncharacterized.

Purpose of the Study:

  • To detect and characterize the radical hydrogen tetrasulfide (HS(4)) in the gas phase.
  • To investigate the structures and energies of HS(4) in different oxidation states (+/0/-) using computational methods.
  • To report the first detection of HS(4)(-) and its parent acid, H(2)S(4).

Main Methods:

  • Gas-phase detection using mass spectrometric experiments.
  • Ab initio quantum chemical calculations for structure and energy investigations.
  • Analysis of radical stability and dissociation pathways.

Main Results:

  • The radical HS(4), featuring an open-chain HSSSS structure with three sulfur-sulfur bonds, was successfully detected.
  • Computational studies determined the relative energies of HS(4) in its radical, cationic, and anionic forms.
  • HS(4) was found to be stable, with a dissociation energy of 23 kcal mol(-1) against fragmentation into S(2) and HS(2).
  • The conjugate base, HS(4)(-), of the strong acid H(2)S(4), was identified for the first time.

Conclusions:

  • The existence and stability of the HS(4) radical have been experimentally confirmed.
  • Ab initio calculations provide detailed structural and energetic insights into HS(4) and its related species.
  • The discovery of HS(4)(-) expands the known family of sulfur-hydrogen anions and provides evidence for the strong acid H(2)S(4).