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Carbonic acid: from polyamorphism to polymorphism.

Katrin Winkel1, Wolfgang Hage, Thomas Loerting

  • 1Institute of General, Inorganic, and Theoretical Chemistry, University of Innsbruck, A-6020 Innsbruck, Austria.

Journal of the American Chemical Society
|October 20, 2007
PubMed
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Two amorphous forms of carbonic acid (H2CO3) were identified, exhibiting distinct structural states and phase transitions to crystalline polymorphs. These findings reveal polyamorphism in carbonic acid, with amorphous states pre-structuring crystalline forms.

Area of Science:

  • Chemistry
  • Materials Science
  • Spectroscopy

Background:

  • Carbonic acid (H2CO3) is a key molecule in various chemical and biological systems.
  • Understanding its structural states, including amorphous and crystalline forms, is crucial for comprehending its behavior.

Purpose of the Study:

  • To investigate the formation and structural properties of amorphous carbonic acid.
  • To explore the phase transitions between amorphous and crystalline states of carbonic acid.
  • To elucidate the phenomenon of polyamorphism in carbonic acid.

Main Methods:

  • Sequential deposition of KHCO3 and HCl solutions (methanolic or aqueous) on a CsI window at 78 K.
  • Heating samples in vacuum from 78 to 230 K.
  • Analysis using Fourier transform infrared (FTIR) spectroscopy.

Related Experiment Videos

  • Confirmation of amorphous nature and structural states using powder X-ray diffraction.

    • Main Results:

    • Two distinct amorphous states of carbonic acid (H2CO3) were formed, dependent on the solvent (methanol or water).
    • FTIR spectra indicated that the H-bond connectivity and conformational states of crystalline alpha- and beta-H2CO3 were largely present in the amorphous precursors.
    • Powder X-ray diffraction confirmed the amorphous nature and distinct structural differences between the two amorphous H2CO3 forms.
    • The study identified polyamorphism in carbonic acid, where two distinct crystalline states are linked to two distinct amorphous states.

    Conclusions:

    • Carbonic acid exhibits polyamorphism, with two distinct amorphous states transitioning to corresponding crystalline polymorphs.
    • The structural motifs present in the amorphous states are retained in the crystalline forms, suggesting pre-structuring.
    • The observed polyamorphism and the connection between amorphous and crystalline states are unique and may involve a first-order-like phase transition.