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Title: Investigation of trimethylacetic acid adsorption on stoichiometric and oxygen-deficient CeO2 (111) surfaces

Abstract

We studied the interactions between the carboxylate anchoring group from trimethylacetic acid (TMAA) and CeO2(111) surfaces as a function of oxygen stoichiometry using in situ X-ray photoelectron spectroscopy (XPS). The stoichiometric CeO2(111) surface was obtained by annealing the thin film under 2.0 × 10–5 Torr of oxygen at ~550 °C for 30 min. In order to reduce the CeO2(111) surface, the thin film was annealed under ~5.0 × 10–10 Torr vacuum conditions at 550 °C, 650 °C, 750 °C and 850 °C for 30 min to progressively increase the oxygen defect concentration on the surface. The saturated TMAA coverage on the CeO2(111) surface determined from XPS elemental composition is found to increase with increasing oxygen defect concentration. This is attributed to the increase of under-coordinated cerium sites on the surface with the increase in the oxygen defect concentrations. Furthermore, XPS results were in agreement with periodic density functional theory (DFT) calculations and indicate a stronger binding between the carboxylate group from TMAA and the oxygen deficient CeO2–δ(111) surface through dissociative adsorption.

Authors:
 [1];  [2];  [1];  [3];  [4];  [5];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Shaanxi Normal Univ., Xi'an (China)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Ahmedabad Univ. (India)
  4. Shaanxi Normal Univ., Xi'an (China)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1329595
Report Number(s):
LA-UR-16-20620
Journal ID: ISSN 1463-9076; PPCPFQ
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Volume: 18; Journal Issue: 23; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Inorganic and Physical Chemistry

Citation Formats

Sanghavi, Shail, Wang, Weina, Nandasiri, Manjula I., Karakoti, Ajay S., Wang, Wenliang, Yang, Ping, and Thevuthasan, S. Investigation of trimethylacetic acid adsorption on stoichiometric and oxygen-deficient CeO2 (111) surfaces. United States: N. p., 2016. Web. doi:10.1039/C6CP00855K.
Sanghavi, Shail, Wang, Weina, Nandasiri, Manjula I., Karakoti, Ajay S., Wang, Wenliang, Yang, Ping, & Thevuthasan, S. Investigation of trimethylacetic acid adsorption on stoichiometric and oxygen-deficient CeO2 (111) surfaces. United States. https://doi.org/10.1039/C6CP00855K
Sanghavi, Shail, Wang, Weina, Nandasiri, Manjula I., Karakoti, Ajay S., Wang, Wenliang, Yang, Ping, and Thevuthasan, S. 2016. "Investigation of trimethylacetic acid adsorption on stoichiometric and oxygen-deficient CeO2 (111) surfaces". United States. https://doi.org/10.1039/C6CP00855K. https://www.osti.gov/servlets/purl/1329595.
@article{osti_1329595,
title = {Investigation of trimethylacetic acid adsorption on stoichiometric and oxygen-deficient CeO2 (111) surfaces},
author = {Sanghavi, Shail and Wang, Weina and Nandasiri, Manjula I. and Karakoti, Ajay S. and Wang, Wenliang and Yang, Ping and Thevuthasan, S.},
abstractNote = {We studied the interactions between the carboxylate anchoring group from trimethylacetic acid (TMAA) and CeO2(111) surfaces as a function of oxygen stoichiometry using in situ X-ray photoelectron spectroscopy (XPS). The stoichiometric CeO2(111) surface was obtained by annealing the thin film under 2.0 × 10–5 Torr of oxygen at ~550 °C for 30 min. In order to reduce the CeO2(111) surface, the thin film was annealed under ~5.0 × 10–10 Torr vacuum conditions at 550 °C, 650 °C, 750 °C and 850 °C for 30 min to progressively increase the oxygen defect concentration on the surface. The saturated TMAA coverage on the CeO2(111) surface determined from XPS elemental composition is found to increase with increasing oxygen defect concentration. This is attributed to the increase of under-coordinated cerium sites on the surface with the increase in the oxygen defect concentrations. Furthermore, XPS results were in agreement with periodic density functional theory (DFT) calculations and indicate a stronger binding between the carboxylate group from TMAA and the oxygen deficient CeO2–δ(111) surface through dissociative adsorption.},
doi = {10.1039/C6CP00855K},
url = {https://www.osti.gov/biblio/1329595}, journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
issn = {1463-9076},
number = 23,
volume = 18,
place = {United States},
year = {Thu May 12 00:00:00 EDT 2016},
month = {Thu May 12 00:00:00 EDT 2016}
}

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