Pressure-Induced Polymerization of Diiodobutadiyne in Assembled Cocrystals.

Diiodobutadiyne forms cocrystals with bis(pyridyl)oxalamides in which the diyne alignment is near the ideal parameters for topochemical polymerization to the ordered conjugated polymer, poly-(diiododiacetylene) (PIDA). Nonetheless, previous efforts to induce polymerization in these samples via heat...

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Publicado en:Journal of the American Chemical Society Vol. 130; no. 13; pp. 4415 - 4421
Autores principales: Wilhelm, Christopher, Boyd, Stephen A., Chawda, Samrat, Fowler, Frank W., Goroff, Nancy S., Halada, Gary P., Grey, Clare P., Lauher, Joseph W., Liang Luo, Martin, C. David, Parise, John B., Tarabrella, Cathy, Webb, Jeffrey A.
Formato: Artículo
Publicado: American Chemical Society 4/2/2008
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 4/2/2008
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      pub: American Chemical Society
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        10.1021/ja0782910
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        atl: Pressure-Induced Polymerization of Diiodobutadiyne in Assembled Cocrystals.
      aug:
        au:
          Wilhelm, Christopher
          Boyd, Stephen A.
          Chawda, Samrat
          Fowler, Frank W.
          Goroff, Nancy S.
          Halada, Gary P.
          Grey, Clare P.
          Lauher, Joseph W.
          Liang Luo
          Martin, C. David
          Parise, John B.
          Tarabrella, Cathy
          Webb, Jeffrey A.
        affil:
          Department of Chemistry, State University of New York, Stony Brook, New York 11794-3400
          Department of Geosciences, State University of New York, Stony Brook, New York 11794-2100
          Department of Materials Science and Engineering, State University of New York, Stony Brook, New York 11794-2275
      su:
        Polymerization
        Crystals
        Polymers
        Optical diffraction
        Chemical reactions
      sug:
        subj:
          Polymerization
          Crystals
          Polymers
          Optical diffraction
          Chemical reactions
      ab: Diiodobutadiyne forms cocrystals with bis(pyridyl)oxalamides in which the diyne alignment is near the ideal parameters for topochemical polymerization to the ordered conjugated polymer, poly-(diiododiacetylene) (PIDA). Nonetheless, previous efforts to induce polymerization in these samples via heat or irradiation were unsuccessful. We report here the successful ordered polymerization of diiodobutadiyne in these cocrystals, by subjecting them to high external pressure (0.3-10 GPa). At the lower end of the pressure range, the samples contain primarily monomer, as demonstrated by X-ray diffraction studies, but some polymerization does occur, leading to a pronounced color change from colorless to blue and to the development of intense Raman peaks at 962, 1394, and 2055 cm, corresponding to the poly-(diacetylene). At higher pressures, the samples turn black and contain primarily polymer, as determined by solid-state NMR and Raman spectroscopy. Both density functional theory calculations (B3LYP/LanL2DZ) and comparisons to authentic samples of PIDA have confirmed the data analysis.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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