Palladium Vacataporphyrin Reveals Conformational Rearrangements Involving Hückel and Möbius Macrocyclic Topologies.

5,10,15,20-Tetraaryl-21-vacataporphyrin (butadieneporphyrin, an annulene-porphyrin hybrid) which contains a vacant space instead of heteroatomic bridge acts as a ligand toward palladium(II). The metal ion of square-planar coordination geometry is firmly held via three pyrrolic nitrogen atoms where t...

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Published in:Journal of the American Chemical Society Vol. 130; no. 19; pp. 6182 - 6196
Main Authors: Pacholska-Dudziak, Ewa, Skonieczny, Janusz, Pawlicki, Miłosz, Szterenberg, Ludmiła, Ciunik, Zbigniew, Latos-Grażyński, Lechosław
Format: Article
Published: American Chemical Society 5/14/2008
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Online Access:View this record in EBSCOhost
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      dt: 5/14/2008
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      pub: American Chemical Society
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        10.1021/ja711039c
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        atl: Palladium Vacataporphyrin Reveals Conformational Rearrangements Involving Hückel and Möbius Macrocyclic Topologies.
      aug:
        au:
          Pacholska-Dudziak, Ewa
          Skonieczny, Janusz
          Pawlicki, Miłosz
          Szterenberg, Ludmiła
          Ciunik, Zbigniew
          Latos-Grażyński, Lechosław
        affil: Department of Chemistry, University of Wrocław, Joliot-Curie 14, 50 383 Wrocław, Poland
      su:
        Physical & theoretical chemistry research
        Palladium
        Conformational analysis
        Macrocyclic compounds
        Nuclear magnetic resonance
        Density functionals
      sug:
        subj:
          Physical & theoretical chemistry research
          Palladium
          Conformational analysis
          Macrocyclic compounds
          Nuclear magnetic resonance
          Density functionals
      ab: 5,10,15,20-Tetraaryl-21-vacataporphyrin (butadieneporphyrin, an annulene-porphyrin hybrid) which contains a vacant space instead of heteroatomic bridge acts as a ligand toward palladium(II). The metal ion of square-planar coordination geometry is firmly held via three pyrrolic nitrogen atoms where the fourth coordination place is occupied by a monodentate ligand or by an annulene part of vacataporphyrin. The macrocycle reveals the unique structural flexibility triggered by coordination of palladium. The structural rearrangements engage the C(20)C(1)C(2)C(3)C(4)C(5) annulene fragment which serves as a linker between two pyrrolic rings of vacataporphyrin albeit the significant ruffling of the tripyrrolic block is also of importance. Two fundamental modes of interactions between the palladium ion and annulene moiety have been recognized. The first one resembles an η-type interaction and involves the C(2)C(3) unit of the butadiene part. Alternatively the profound conformational adjustments allowed an in-plane coordination through the deprotonated trigonally hybridized C(2) center of butadiene. The coordinated vacataporphyrin acquires Hückel or extremely rare Möbius topologies readily reflected by spectroscopic properties. The palladium vacataporphyrin complexes reveal Hückel aromaticity or Möbius antiaromaticity of [18]annulene applying the butadiene fragment of vacataporphyrin as a topology selector. The properties of specific conformers were determined using H NMR and density functional theory calculations.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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