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Geometrical Structures of Partially Oxidized Rhodium Cluster Cations, Rh 6 O m + (m = 4, 5, 6), Revealed by Infrared Multiple Photon Dissociation Spectroscopy.
Journal of Physical Chemistry. A 2016 November 4
Infrared multiple photon dissociation (IRMPD) spectra of Rh6 Om + (m = 4-10) are obtained in the 300-1000 cm-1 spectral range using the free electron laser for infrared experiments (FELIX) via dissociation of Rh6 Om + or Rh6 Om + -Ar complexes. The spectra are compared with the calculated spectra of several stable geometries obtained by density functional theory (DFT) structural optimization. The spectrum for Rh6 O4 + shows prominent bands at 620 and 690 cm-1 and is assigned to a capped-square pyramidal Rh atom geometry with three bridging O atoms and one O atom in a hollow site. Rh6 O5 + displays bands at 460, 630, 690, and 860 cm-1 and has a prismatic Rh geometry with three bridging O atoms and two O atoms in a hollow site. Rh6 O6 + shows three intense bands around 600-750 cm-1 and multiple weak bands in the range of 350-550 cm-1 . This species has a prismatic Rh geometry with four bridging O atoms and two O atoms in a hollow site. Considering that Rh6 Om + (m ≤ 3) adopts tetragonal bipyramidal Rh6 structures, the change at m = 4 to capped bipyramidal and at m = 5 to prismatic geometries results in a reduction of the number of triangular hollow sites. Since NO preferentially binds on a triangular hollow site through the N atom, the geometry change lowers the possibility of NO dissociative adsorption.
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