Investigating the Role of Solvent-Solute Interaction in Crystal Nucleation of Salicylic Acid from Organic Solvents.

In previous work, it has been shown that the crystal nucleation of salicylic acid (SA) in different solvents becomes increasingly more difficult in the order: chloroform, ethyl acetate acetonitrile, acetone, methanol, and acetic acid. In the present work, vibration spectroscopy, calorimetric measure...

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Published in:Journal of the American Chemical Society Vol. 136; no. 33; pp. 11664 - 11674
Main Authors: Khamar, Dikshitkumar, Zeglinski, Jacek, Mealey, Donal, Rasmuson, Åke C.
Format: Article
Published: American Chemical Society 8/20/2014
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Online Access:View this record in EBSCOhost
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      dt: 8/20/2014
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        10.1021/ja503131w
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        atl: Investigating the Role of Solvent-Solute Interaction in Crystal Nucleation of Salicylic Acid from Organic Solvents.
      aug:
        au:
          Khamar, Dikshitkumar
          Zeglinski, Jacek
          Mealey, Donal
          Rasmuson, Åke C.
        affil:
          Materials and Surface Science Institute, Department of Chemical and Environmental Science, University of Limerick, Limerick, Ireland
          Department of Chemical Engineering and Technology, KTH Royal Institute of Technology, SE-100 44 Stockholm, Sweden
      su:
        Nucleation
        Crystal growth
        Salicylic acid
        Solution (Chemistry)
        Solvent testing
        Vibrational spectra
        Calorimetry
        Density functional theory
      sug:
        subj:
          Nucleation
          Crystal growth
          Salicylic acid
          Solution (Chemistry)
          Solvent testing
          Vibrational spectra
          Calorimetry
          Density functional theory
      ab: In previous work, it has been shown that the crystal nucleation of salicylic acid (SA) in different solvents becomes increasingly more difficult in the order: chloroform, ethyl acetate acetonitrile, acetone, methanol, and acetic acid. In the present work, vibration spectroscopy, calorimetric measurements, and density functional theory (DFT) calculations are used to reveal the underlying molecular mechanisms. Raman and infrared spectra suggest that SA exists predominately as dimers in chloroform, but in the other five solvents there is no clear evidence of dimerization. In all solvents, the shift in the SA carbonyl peak reflecting the strength in the solvent—solute interaction is quite well correlated to the nucleation ranking. This shift is corroborated by DFT calculated energies of binding one solvent molecule to the carboxyl group of SA. An even better correlation of the influence of the solvent on the nucleation is provided by DFT calculated energy of binding the complete first solvation shell to the SA molecule. These solvation shell binding energies are corroborated by the enthalpy of solvent—solute interaction as estimated from experimentally determined enthalpy of solution and calculated enthalpy of cavity formation using the scaled particle theory. The different methods reveal a consistent picture and suggest that the stronger the solvent binds to the SA molecule in solution, the slower the nucleation becomes.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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