Density functional calculations and IR reflection absorption spectroscopy on the interaction of SO2 with oxide-supported Pd nanoparticles

Journal article
(Original article)


Publication Details

Author(s): Luckas N, Vines Solana F, Happel M, Desikusumastuti A, Libuda J, Görling A
Journal: Journal of Physical Chemistry C
Publisher: American Chemical Society
Publication year: 2010
Volume: 114
Journal issue: 32
Pages range: 13813-13824
ISSN: 1932-7447
eISSN: 1932-7455


Abstract


A systematic study on the interaction of sulfur dioxide (SO) on BaO-supported Pd nanoparticles has been carried out using suitable models and state-of-the-art density functional (DF) calculations. Detailed information concerning the structure and energetics of the different conformations of adsorbed SO is provided as a function of coverage together with calculated infrared reflection absorption spectroscopy (IRAS) spectra. SO may adsorb on Pd(111) in several conformations, some active, η-SO and η-S , and others inactive in IRAS, η-SO O. SO is found to attach stronger to Pd nanoparticle edges and corners, a fact intimately related to catalyst poisoning by site blocking. On Pd nanoparticles, SO is found to preferably adopt adsorption conformations that depend on the specific region on the nanoparticle, thus adding site specificity to vibrational recognition. Molecular beam experiments and IRAS have been performed on a single-crystal-based Pd/BaAlO/NiAl(110) model NO storage and reduction catalyst and its individual components. SO formation on the oxide components, evolution of a SO multilayer, and adsorption of SO on BaO or Pd nanoparticles is linked to DF calculations. The effect of cation intermixing in the oxide support and overlap of absorption bands on the unequivocal discrimination of signals are discussed. © 2010 American Chemical Society.



FAU Authors / FAU Editors

Görling, Andreas Prof. Dr.
Lehrstuhl für Theoretische Chemie
Happel, Markus
Lehrstuhl für Physikalische Chemie II
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Luckas, Nicola
Lehrstuhl für Theoretische Chemie


Additional Organisation
Exzellenz-Cluster Engineering of Advanced Materials


Research Fields

D Catalytic Materials
Exzellenz-Cluster Engineering of Advanced Materials
A3 Multiscale Modeling and Simulation
Exzellenz-Cluster Engineering of Advanced Materials


How to cite

APA:
Luckas, N., Vines Solana, F., Happel, M., Desikusumastuti, A., Libuda, J., & Görling, A. (2010). Density functional calculations and IR reflection absorption spectroscopy on the interaction of SO2 with oxide-supported Pd nanoparticles. Journal of Physical Chemistry C, 114(32), 13813-13824. https://dx.doi.org/10.1021/jp105097z

MLA:
Luckas, Nicola, et al. "Density functional calculations and IR reflection absorption spectroscopy on the interaction of SO2 with oxide-supported Pd nanoparticles." Journal of Physical Chemistry C 114.32 (2010): 13813-13824.

BibTeX: 

Last updated on 2019-06-08 at 09:05