Surface-assisted dehydrogenative homocoupling of porphine molecules

J Am Chem Soc. 2014 Jul 2;136(26):9346-54. doi: 10.1021/ja501680n. Epub 2014 Jun 23.

Abstract

The templated synthesis of porphyrin dimers, oligomers, and tapes has recently attracted considerable interest. Here, we introduce a clean, temperature-induced covalent dehydrogenative coupling mechanism between unsubstituted free-base porphine units yielding dimers, trimers, and larger oligomers directly on a Ag(111) support under ultrahigh-vacuum conditions. Our multitechnique approach, including scanning tunneling microscopy, near-edge X-ray absorption fine structure and photoelectron spectroscopy complemented by theoretical modeling, allows a comprehensive characterization of the resulting nanostructures and sheds light on the coupling mechanism. We identify distinct coupling motifs and report a decrease of the electronic gap and a modification of the frontier orbitals directly associated with the formation of triply fused dimeric species. This new on-surface homocoupling protocol yields covalent porphyrin nanostructures addressable with submolecular resolution and provides prospective model systems towards the exploration of extended oligomers with tailored chemical and physical properties.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Dimerization
  • Microscopy, Scanning Tunneling
  • Nanostructures / chemistry
  • Photoelectron Spectroscopy
  • Porphyrins / chemistry*
  • Porphyrins / metabolism
  • Silver / chemistry
  • X-Ray Absorption Spectroscopy

Substances

  • Porphyrins
  • Silver
  • porphine