Search for a Predicted Hydrogen Bonding Motif – A Multidisciplinary Investigation into the Polymorphism of 3-Azabicyclo[3.3.1]nonane-2,4-dione.

The predictions of the crystal structure of 3-azabicyclo[3.3.1]nonane-2,4-dione submitted in the 2001 international blind test of crystal structure prediction (CSP2001) led to the conclusion that crystal structures containing an alternative hydrogen bonded dimer motif were energetically competitive...

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Publicado en:Journal of the American Chemical Society Vol. 129; no. 12; pp. 3649 - 3658
Autores principales: Hulme, Ashley T., Johnston, Andrea, Florence, Alastair J., Fernandes, Phillipe, Shankland, Kenneth, Bedford, Cohn T., Welch, Gareth W. A., Sadiq, Ghazala, Haynes, Delia A., Samuel Motherwell, W. D., Tocher, Derek A., Price, Sarah L.
Formato: Artículo
Publicado: American Chemical Society 3/28/2007
Materias:
Acceso en línea:Ver este registro en EBSCOhost
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      dt: 3/28/2007
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      pub: American Chemical Society
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        24961709
        10.1021/ja0687466
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        atl: Search for a Predicted Hydrogen Bonding Motif – A Multidisciplinary Investigation into the Polymorphism of 3-Azabicyclo[3.3.1]nonane-2,4-dione.
      aug:
        au:
          Hulme, Ashley T.
          Johnston, Andrea
          Florence, Alastair J.
          Fernandes, Phillipe
          Shankland, Kenneth
          Bedford, Cohn T.
          Welch, Gareth W. A.
          Sadiq, Ghazala
          Haynes, Delia A.
          Samuel Motherwell, W. D.
          Tocher, Derek A.
          Price, Sarah L.
        affil:
          University College London
          University of Strathclyde
          CCLRC Rutherford Appleton Laboratory
          University of Manchester
          Cambridge Crystallographic Data Centre
          School of Chemistry, University of KwaZulu-Natal
      su:
        Hydrogen bonding
        Polymorphism (Crystallography)
        Solution (Chemistry)
        Diffraction patterns
        Dimers
        Fourier transform infrared spectroscopy
        Physical & theoretical chemistry research
      sug:
        subj:
          Hydrogen bonding
          Polymorphism (Crystallography)
          Solution (Chemistry)
          Diffraction patterns
          Dimers
          Fourier transform infrared spectroscopy
          Physical & theoretical chemistry research
      ab: The predictions of the crystal structure of 3-azabicyclo[3.3.1]nonane-2,4-dione submitted in the 2001 international blind test of crystal structure prediction (CSP2001) led to the conclusion that crystal structures containing an alternative hydrogen bonded dimer motif were energetically competitive with the known catemer-based structure. Here we report an extensive search for a dimer-based crystal structure. Using an automated polymorph screen a new catemer-based metastable polymorph (form 2) and two new catemer-based solvates were found, and concurrent thermal studies reproduced form 2 and identified a plastic phase (form 3), whose powder X-ray diffraction pattern was consistent with the cubic space group I2 (a = 7.5856(1) Å). Computational studies on the monomer showed that the imide NH was a weak hydrogen bond donor, rationalizing the occurrence of the plastic phase which involved the breaking of all hydrogen bonds, and modeling of small clusters showed that dimers could easily reorganize to give the catemer. FTIR spectra confirmed the weakness of the hydrogen bond, with the solute showing no self-assembly in solution. It is concluded that the weakness of the NH donor, coupled with the globular shape of the molecule, allows unusually facile transformation between alternative hydrogen bonding motifs during aggregation and nucleation.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2007
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