Single and dual cation sites in zeolites: theoretical calculations and FTIR spectroscopic studies on CO adsorption on K-FER

J Phys Chem B. 2006 Nov 16;110(45):22542-50. doi: 10.1021/jp0631331.

Abstract

Interaction of CO with K-FER zeolite was investigated by a combination of variable-temperature IR spectroscopy and computational study. Calculations were performed using omega(CO)/r(CO) correlation method in combination with a periodic density functional theory model. On the basis of agreement between experimental and calculated results, the following carbonyl complexes were identified: (i) mono- and dicarbonyl C-down complexes on single K(+) sites characterized by IR absorption bands at 2163 and 2161 cm(-1), respectively; (ii) complexes formed by CO bridging two K(+) ions separated by about 7-8 A (dual sites) characterized by a band at 2148 cm(-1); and (iii) isocarbonyl (O-down) complexes characterized by a band at 2116 cm(-1). The bridged carbonyl complexes on dual K(+) sites are about 5 kJ/mol more stable than monodentate (monocarbonyl) CO complexes. The C-O stretching frequency of monocarbonyl species in K-FER depends on K(+) location in the zeolite, and not on K(+) coordination to the framework. A combination of theoretical calculations using a periodic density functional model and experimental results showed formation of two types of monocarbonyls. The most abundant type appears at 2163 cm(-1), and the less abundant one at 2172 cm(-1). These experimentally determined wavenumber values coincide, within +/-2 cm(-1), with those derived from theoretical calculations.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Adsorption
  • Algorithms*
  • Binding Sites
  • Carbon / chemistry
  • Cations / chemistry
  • Models, Molecular
  • Oxygen / chemistry
  • Potassium / chemistry*
  • Spectroscopy, Fourier Transform Infrared / methods*
  • Thermodynamics
  • Zeolites / analysis*
  • Zeolites / chemistry*

Substances

  • Cations
  • Zeolites
  • Carbon
  • Potassium
  • Oxygen