Synthesis and supramolecular properties of molecular clips with anthracene sidewalls

Chemistry. 2005 May 20;11(11):3363-74. doi: 10.1002/chem.200401257.

Abstract

Novel molecular clips with anthracene sidewalls (1 a-c) were synthesized; they form stable host-guest complexes with a variety of electron-deficient aromatic and quinoid molecules. According to single-crystal structure analyses of clip 1 c and 1,2,4,5-tetracyanobenzene (TCNB) complex 14@1 b, the clips' anthracene sidewalls have to be compressed substantially during the complex formation to provide attractive pi-pi interactions between the aromatic guest molecule and the two anthracene sidewalls in the complex. The compression and expansion of aromatic sidewalls are calculated by molecular mechanics to be low-energy processes, so the energy required for compression of the anthracene sidewalls during complex formation is apparently overcompensated by the gain in energy resulting from the attractive pi-pi interactions. The finding that complexes of the clips 1 a-c are more stable than those of the corresponding clips 2 a-c can be explained in terms of the larger van der Waals contact surfaces of the anthracene sidewalls in 1 a-c (relative to the naphthalene sidewalls in 2 a-c). Color changes resulting from charge-transfer (CT) bands are observed in complex formation by 1 a-c: from colorless to red or purple with TCNB (14), and from yellow to green with 2,4,7-trinitro-9-fluorenone TNF (17). Independently, the host 1 b and guest 14 fluoresce from their respective excited singlet states, whilst in the complex 14@1 b the charge-transfer state quenches the higher-energy singlet states of the two components, and as a result luminescence is only observed from this new CT state. To the best of our knowledge, complex 14@1 b is the first example of CT luminescence from a host-guest complex. The binding constant determined for the formation of the TCNB complex 14@1 b from a UV/Vis titration experiment (Ka = 12 400 m(-1)) agrees well with the value (K(a) = 12 800 m(-1)) obtained by 1H NMR titration.

Publication types

  • Comparative Study
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anthracenes / chemical synthesis*
  • Anthracenes / chemistry
  • Benzene Derivatives / chemistry*
  • Crystallography, X-Ray
  • Fluorenes / chemistry*
  • Luminescent Measurements
  • Magnetic Resonance Spectroscopy
  • Models, Molecular
  • Monte Carlo Method
  • Naphthalenes / chemical synthesis*
  • Naphthalenes / chemistry
  • Nitriles / chemistry*
  • Quantum Theory
  • Spectrophotometry, Infrared
  • Spectrophotometry, Ultraviolet

Substances

  • 1,2,4,5-tetracyanobenzene
  • Anthracenes
  • Benzene Derivatives
  • Fluorenes
  • Naphthalenes
  • Nitriles
  • 2,4,7-trinitrofluorenone