Self-assembly of bidentate ligands for combinatorial homogeneous catalysis based on an A-T base-pair model.

نویسندگان

  • Bernhard Breit
  • Wolfgang Seiche
چکیده

A new concept for generation of chelating ligand libraries for homogeneous metal complex catalysis based on self-assembly is presented. Thus, self-assembly of structurally simple monodentate ligands in order to give structurally more complex bidentate ligands is achieved employing hydrogen bonding. Based on this concept and on the 2-pyridone/hydroxypyridine tautomeric system, a new rhodium catalyst was identified which operated with excellent activity and regioselectivity upon hydroformylation of terminal alkenes. In order to generate defined unsymmetrical heterodimeric ligands, an A–T base pair analog—the aminopyridine/isoquinolone system—was developed which allows for complementary hydrogen bonding. Based on this platform, a 4 × 4 phosphine ligand library was screened in the course of the rhodium-catalyzed hydroformylation of 1-octene. A catalyst operating with outstanding activity and regioselectivity in favor of the linear aldehyde was discovered.

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Catalysts through self-assembly for combinatorial homogeneous catalysis*

Inspired by the principle of DNA base-pairing, a new concept for the self-assembly of molecular catalysts is described herein. Thus, employing A–T analogous complementary hydrogen-bonding templates, self-assembly of monodentate to bidentate ligands in the coordination sphere of a transition-metal salt occurs to give defined self-assembly catalysts. This approach is intrinsically combinatorial a...

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عنوان ژورنال:
  • Angewandte Chemie

دوره 44 11  شماره 

صفحات  -

تاریخ انتشار 2005