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Title: Environmentally benign synthesis of a PGM-free catalyst for low temperature CO oxidation

Abstract

Dopants enhance the catalytic properties of ceria. However, conventional techniques for synthesizing doped ceria have limitations in terms of structural homogeneity, surface area, and catalytic activity of the resulting oxide. Use of toxic and corrosive chemicals presents further challenges. The sol-gel method described in this work provides a facile approach for incorporating high concentrations of dopants in a uniform, high surface area structure, yielding excellent catalytic activity. Addition of polyvinylpyrrolidone (PVP) complexing agent prevents the segregation of cerium and dopant atoms during synthesis. Surface areas up to 179 m2/g are achieved, which represents a substantial improvement over doped ceria produced through coprecipitation, solution combustion, or melt-synthesis methods. The resulting powders exhibit dramatically improved CO oxidation activity (T90 = 132 °C for 3.2 wt% Cu-CeO2 compared to 274 °C for a 2 wt% Pt-Al2O3 reference catalyst). First principles calculations suggest a Mars Van Krevelen mechanism, which is facilitated by dopants causing oxygen vacancies.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [2];  [4];  [4];  [2];  [4]; ORCiD logo [5];  [6]; ORCiD logo [2]
  1. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering and Center for Microengineered Materials
  2. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering and Center for Microengineered Materials
  3. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology; Jingdezhen Ceramic Inst. (China). Dept. of Material Science and Engineering
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology; Fuzhou Univ. (China). State Key Lab. of Photocatalysis on Energy and Environment, College of Chemistry
  6. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1608286
Alternate Identifier(s):
OSTI ID: 1580316
Grant/Contract Number:  
AC02-76SF00515; FG02-05ER15712; FA9550-18-1-0413
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis B: Environmental
Additional Journal Information:
Journal Volume: 264; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Dopant; Ceria; CO oxidation; Polyvinylpyrrolidone; Sol-gel synthesis

Citation Formats

Riley, Christopher, Canning, Griffin, De La Riva, Andrew, Zhou, Shulan, Peterson, Eric, Boubnov, Alexey, Hoffman, Adam, Tran, Minh, Bare, Simon R., Lin, Sen, Guo, Hua, and Datye, Abhaya. Environmentally benign synthesis of a PGM-free catalyst for low temperature CO oxidation. United States: N. p., 2019. Web. https://doi.org/10.1016/j.apcatb.2019.118547.
Riley, Christopher, Canning, Griffin, De La Riva, Andrew, Zhou, Shulan, Peterson, Eric, Boubnov, Alexey, Hoffman, Adam, Tran, Minh, Bare, Simon R., Lin, Sen, Guo, Hua, & Datye, Abhaya. Environmentally benign synthesis of a PGM-free catalyst for low temperature CO oxidation. United States. https://doi.org/10.1016/j.apcatb.2019.118547
Riley, Christopher, Canning, Griffin, De La Riva, Andrew, Zhou, Shulan, Peterson, Eric, Boubnov, Alexey, Hoffman, Adam, Tran, Minh, Bare, Simon R., Lin, Sen, Guo, Hua, and Datye, Abhaya. Fri . "Environmentally benign synthesis of a PGM-free catalyst for low temperature CO oxidation". United States. https://doi.org/10.1016/j.apcatb.2019.118547. https://www.osti.gov/servlets/purl/1608286.
@article{osti_1608286,
title = {Environmentally benign synthesis of a PGM-free catalyst for low temperature CO oxidation},
author = {Riley, Christopher and Canning, Griffin and De La Riva, Andrew and Zhou, Shulan and Peterson, Eric and Boubnov, Alexey and Hoffman, Adam and Tran, Minh and Bare, Simon R. and Lin, Sen and Guo, Hua and Datye, Abhaya},
abstractNote = {Dopants enhance the catalytic properties of ceria. However, conventional techniques for synthesizing doped ceria have limitations in terms of structural homogeneity, surface area, and catalytic activity of the resulting oxide. Use of toxic and corrosive chemicals presents further challenges. The sol-gel method described in this work provides a facile approach for incorporating high concentrations of dopants in a uniform, high surface area structure, yielding excellent catalytic activity. Addition of polyvinylpyrrolidone (PVP) complexing agent prevents the segregation of cerium and dopant atoms during synthesis. Surface areas up to 179 m2/g are achieved, which represents a substantial improvement over doped ceria produced through coprecipitation, solution combustion, or melt-synthesis methods. The resulting powders exhibit dramatically improved CO oxidation activity (T90 = 132 °C for 3.2 wt% Cu-CeO2 compared to 274 °C for a 2 wt% Pt-Al2O3 reference catalyst). First principles calculations suggest a Mars Van Krevelen mechanism, which is facilitated by dopants causing oxygen vacancies.},
doi = {10.1016/j.apcatb.2019.118547},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 264,
place = {United States},
year = {2019},
month = {12}
}