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Title: Reactivity of a Thick BaO Film Supported on Pt(111): Adsorption and Reaction of NO2, H2O and CO2

Abstract

Reactions of NO2, H2O, and CO2 with a thick (> 20 MLE) BaO film supported on Pt(111) were studied with temperature programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS). NO2 reacts with a thick BaO to form surface nitrite-nitrate ion pairs at 300 K, while only nitrates form at 600 K. In the thermal decomposition process of nitrite–nitrate ion pairs, first nitrites decompose and desorb as NO. Then nitrates decompose in two steps : at lower temperature with the release of NO2 and at higher temperature, nitrates dissociate to NO + O2. The thick BaO layer converts completely to Ba(OH)2 following the adsorption of H2O at 300 K. Dehydration/dehydroxylation of this hydroxide layer can be fully achieved by annealing to 550 K. CO2 also reacts with BaO to form BaCO3 that completely decomposes to regenerate BaO upon annealing to 825 K. However, the thick BaO film cannot be converted completely to Ba(NOx)2 or BaCO3 under the experimental conditions employed in this study.

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
965564
Report Number(s):
PNNL-SA-65964
Journal ID: ISSN 0743-7463; LANGD5; 30469; KC0302010; TRN: US200920%%342
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Langmuir, 25(18):10820-10828
Additional Journal Information:
Journal Volume: 25; Journal Issue: 18; Journal ID: ISSN 0743-7463
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CHEMICAL REACTIONS; NITROGEN DIOXIDE; WATER; CARBON DIOXIDE; BARIUM OXIDES; FILMS; SUBSTRATES; PLATINUM; CHEMICAL REACTION KINETICS; Environmental Molecular Sciences Laboratory

Citation Formats

Mudiyanselage, Kumudu, Yi, Cheol-Woo W, and Szanyi, Janos. Reactivity of a Thick BaO Film Supported on Pt(111): Adsorption and Reaction of NO2, H2O and CO2. United States: N. p., 2009. Web. doi:10.1021/la901371g.
Mudiyanselage, Kumudu, Yi, Cheol-Woo W, & Szanyi, Janos. Reactivity of a Thick BaO Film Supported on Pt(111): Adsorption and Reaction of NO2, H2O and CO2. United States. doi:10.1021/la901371g.
Mudiyanselage, Kumudu, Yi, Cheol-Woo W, and Szanyi, Janos. Tue . "Reactivity of a Thick BaO Film Supported on Pt(111): Adsorption and Reaction of NO2, H2O and CO2". United States. doi:10.1021/la901371g.
@article{osti_965564,
title = {Reactivity of a Thick BaO Film Supported on Pt(111): Adsorption and Reaction of NO2, H2O and CO2},
author = {Mudiyanselage, Kumudu and Yi, Cheol-Woo W and Szanyi, Janos},
abstractNote = {Reactions of NO2, H2O, and CO2 with a thick (> 20 MLE) BaO film supported on Pt(111) were studied with temperature programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS). NO2 reacts with a thick BaO to form surface nitrite-nitrate ion pairs at 300 K, while only nitrates form at 600 K. In the thermal decomposition process of nitrite–nitrate ion pairs, first nitrites decompose and desorb as NO. Then nitrates decompose in two steps : at lower temperature with the release of NO2 and at higher temperature, nitrates dissociate to NO + O2. The thick BaO layer converts completely to Ba(OH)2 following the adsorption of H2O at 300 K. Dehydration/dehydroxylation of this hydroxide layer can be fully achieved by annealing to 550 K. CO2 also reacts with BaO to form BaCO3 that completely decomposes to regenerate BaO upon annealing to 825 K. However, the thick BaO film cannot be converted completely to Ba(NOx)2 or BaCO3 under the experimental conditions employed in this study.},
doi = {10.1021/la901371g},
journal = {Langmuir, 25(18):10820-10828},
issn = {0743-7463},
number = 18,
volume = 25,
place = {United States},
year = {2009},
month = {9}
}