On the site-specificity of polycarbonyl complexes in Cu/zeolites: combined experimental and DFT study

Phys Chem Chem Phys. 2006 Dec 21;8(47):5535-42. doi: 10.1039/b613805e. Epub 2006 Nov 7.

Abstract

The preferred Cu(+) sites and formation of mono-, di-, and tricarbonyl complexes in the Cu-FER were investigated at the periodic density functional theory level and by means of FTIR spectroscopy. The site-specificity of adsorption enthalpies of CO on Cu-FER and of vibrational frequencies of polycarbonyl complexes were investigated for various Cu(+) sites in Cu-FER. Large changes in the Cu(+) interaction with the zeolite framework were observed upon the formation of carbonyl complexes. The dicarbonyl complexes formed on Cu(+) in the main channel or on the intersection of the main and perpendicular channels are stable and both, adsorption enthalpies and CO stretching frequencies are not site-specific. The fraction of Cu(+) ions in the FER cage, that cannot form dicarbonyl can be determined from IR spectra (about 7% for the Cu-FER with Si/Al = 27.5 investigated here). The tricarbonyl complexes can be formed at the Cu(+) ions located at the 8-member ring window at the intersection of main and perpendicular channel. The stability of tricarbonyl complexes is very low (DeltaH degrees (0 K)>or=-4 kJ mol(-1)).

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Carbon Monoxide / chemistry
  • Copper / chemistry*
  • Ion Channels*
  • Models, Chemical
  • Models, Molecular*
  • Molecular Conformation
  • Organometallic Compounds / chemistry*
  • Polycarboxylate Cement / chemistry*
  • Spectroscopy, Fourier Transform Infrared
  • Thermodynamics
  • Zeolites / chemistry*

Substances

  • Ion Channels
  • Organometallic Compounds
  • Polycarboxylate Cement
  • Zeolites
  • polycarbonate
  • Copper
  • Carbon Monoxide