Mechanism of Sulfur Poisoning and Storage: Adsorption and Reaction of SO2 with Stoichiometric and Reduced Ceria Films on Cu(111)

Happel M, Lykhach Y, Tsud N, Skala T, Prince KC, Matolin V, Libuda J (2011)

Publication Status: Published

Publication Type: Journal article

Publication year: 2011

Journal

Journal of Physical Chemistry C American Chemical Society

Publisher: AMER CHEMICAL SOC

Book Volume: 115

Pages Range: 19872-19882

Journal Issue: 40

DOI: 10.1021/jp207014z

Abstract

We have performed a systematic synchrotron radiation photoelectron spectroscopy (SR-PES) study of the interaction of SO2 with stoichiometric CeO2(111) and reduced CeO2-x films supported on Cu(111). Resonant photoelectron spectroscopy (RPES) was utilized to monitor changes in the cerium oxidation states. Adsorption of SO2 at 150 and 300 K results mostly in formation of sulfite (SO32-) species on both reduced and stoichiometric ceria. Other species such as sulfate (SO42-), SO2 chemisorbed at cationic sites, anionic SO2-, atomic sulfur, surface sulfides, and bulk oxy-sulfides were detected. The origin of these species is discussed in relation to the changes in the oxidation state of ceria cations at the surface. The thermal evolution of the species formed upon adsorption at 150 and 300 K was studied systematically on both the stoichiometric and the reduced films. It was found that the sulfite partially desorbs to release SO2 and partially decomposes. In general, the reduced CeO2-x surface was found to be much more active toward cleavage of S-O bonds, as indicated by a higher amount of oxy-sulfide species produced. The decomposition pathways can be monitored via changes of the ceria oxidation state and are discussed in relation to the stoichiometry of the ceria surface.

Authors with CRIS profile

Markus Happel Lehrstuhl für Physikalische Chemie II Yaroslava Lykhach Lehrstuhl für Physikalische Chemie II Jörg Libuda Professur für Physikalische Chemie

Additional Organisation(s)

Exzellenz-Cluster Engineering of Advanced Materials

Involved external institutions

Elettra Sincrotrone Trieste S.C.p.A. IT Italy (IT) Univerzita Karlova v Praze / Charles University in Prague CZ Czech Republic (CZ)

How to cite

APA:

Happel, M., Lykhach, Y., Tsud, N., Skala, T., Prince, K.C., Matolin, V., & Libuda, J. (2011). Mechanism of Sulfur Poisoning and Storage: Adsorption and Reaction of SO2 with Stoichiometric and Reduced Ceria Films on Cu(111). Journal of Physical Chemistry C, 115(40), 19872-19882. https://dx.doi.org/10.1021/jp207014z

MLA:

Happel, Markus, et al. "Mechanism of Sulfur Poisoning and Storage: Adsorption and Reaction of SO2 with Stoichiometric and Reduced Ceria Films on Cu(111)." Journal of Physical Chemistry C 115.40 (2011): 19872-19882.

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