Unexpected Scholl Reaction of 6,7,13,14-Tetraarylbenzo[k]tetraphene: Selective Formation of Five-Membered Rings in Polycyclic Aromatic Hydrocarbons.

Cyclodehydrogenation is a versatile reaction that has enabled the syntheses of numerous polycyclic aromatic hydrocarbons (PAHs). We now describe a unique Scholl reaction of 6,7,13,14-tetraarylbenzo[k]tetraphene, which "unexpectedly" forms five-membered rings accompanying highly selective 1,2-shift o...

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Publicado en:Journal of the American Chemical Society Vol. 138; no. 8; pp. 2602 - 2609
Autores principales: Junzhi Liu, Akimitsu Narita, Silvio Osella, Wen Zhang, Schollmeyer, Dieter, Beljonne, David, Feng, Xinliang, Müllen, Klaus
Formato: Artículo
Publicado: American Chemical Society 3/2/2016
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 3/2/2016
      vid: 138
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      pub: American Chemical Society
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        10.1021/jacs.5b10399
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        atl: Unexpected Scholl Reaction of 6,7,13,14-Tetraarylbenzo[k]tetraphene: Selective Formation of Five-Membered Rings in Polycyclic Aromatic Hydrocarbons.
      aug:
        au:
          Junzhi Liu
          Akimitsu Narita
          Silvio Osella
          Wen Zhang
          Schollmeyer, Dieter
          Beljonne, David
          Feng, Xinliang
          Müllen, Klaus
        affil:
          Max-Planck Institut für Polymerforschung, Ackermannweg 10, 55128 Mainz, Germany
          Laboratory for Chemistry of Novel Materials, University of Mons, Place du Parc 20, B-7000 Mons, Belgium
          Institut für Organische Chemie, Universität Mainz, Düsbergweg 10-14, 55099 Mainz, Germany
          Center for Advancing Electronics Dresden (CFAED) & Department of Chemistry and Food Chemistry, Technische Universität Dresden, 01062 Dresden, Germany
      su:
        Polycyclic aromatic hydrocarbons
        Aryl group
        Single crystals
        Density functional theory
        Optoelectronic devices
      sug:
        subj:
          Polycyclic aromatic hydrocarbons
          Aryl group
          Single crystals
          Density functional theory
          Optoelectronic devices
      ab: Cyclodehydrogenation is a versatile reaction that has enabled the syntheses of numerous polycyclic aromatic hydrocarbons (PAHs). We now describe a unique Scholl reaction of 6,7,13,14-tetraarylbenzo[k]tetraphene, which "unexpectedly" forms five-membered rings accompanying highly selective 1,2-shift of aryl groups. The geometric and optoelectronic nature of the resulting bistetracene analogue with five-membered rings is comprehensively investigated by single-crystal X-ray, NMR, UV-vis absorption, and cyclic voltammetry analyses. Furthermore, a possible mechanism is proposed to account for the selective five-membered-ring formation with the rearrangement of the aryl groups, which can be rationalized by density functional theory (DFT) calculations. The theoretical results suggest that the formation of the bistetracene analogue with five-membered rings is kinetically controlled while an "expected" product with six-membered rings is thermodynamically more favored. These experimental and theoretical results provide further insights into the still controversial mechanism of the Scholl reaction as well as open up an unprecedented entry to extend the variety of PAHs by programing otherwise unpredictable rearrangements during the Scholl reaction.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2016
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