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Title: In operando studies of CO oxidation on epitaxial SrCoO2.5+δ thin films

Journal Article · · APL Materials
DOI:https://doi.org/10.1063/1.5108957· OSTI ID:1560385
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [1];  [5]; ORCiD logo [1]; ORCiD logo [6]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Chung-Ang Univ., Seoul (South Korea)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pusan National Univ., Busan (Korea)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); Empa, Swiss Federal Labs for Materials Science and Technology, Gallen (Switzerland)
  5. Northern Illinois Univ., DeKalb, IL (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
+ Show Author Affiliations

The high abundance and fast kinetics of select transition metal oxide catalysts are attractive features for many chemical and electrochemical device applications. However, the activity of such catalysts can be accompanied by phase instabilities that prevent their widespread usage. Furthermore, complexities associated with variations in phase behavior and oxygen stoichiometry have hindered studies on the true origins of catalytic activity. Here, we explore the interactions between activity, phase stability, and microstructure using in operando synchrotron X-ray techniques and gas chromatography/mass spectroscopy (GCMS) to probe the behavior of model SrCoO2.5+delta (SCO) catalysts. Pulsed laser deposition was used to prepare SCO thin films on (001) SrTiO3, (111) SrTiO3, and pseudocubic (001) DyScO3 substrates. The GCMS catalytic measurements were performed with a custom-built microreactor compatible with a synchrotron X-ray diffractometer at the Advanced Photon Source. The activity for carbon monoxide oxidation was determined as a function of temperature from 500 degrees C to 800 degrees C. We show that the SrCoO2.5+delta films are active for CO oxidation, most likely by direct reaction with lattice oxygen; consequently, the activity was observed to increase as the films become less stable, with the most active film being the one exhibiting the lowest surface and crystal quality. All films decompose at high temperatures, with in operando diffraction indicating the gradual formation of Sr-rich hexagonal and CoO phases. We find that real-time studies of model oxide systems with synchrotron X-rays is a powerful means of gaining insight into the varied processes taking place at catalytic surfaces.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357
OSTI ID:
1560385
Alternate ID(s):
OSTI ID: 1559362; OSTI ID: 1569463
Journal Information:
APL Materials, Vol. 7, Issue 8; ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

References (27)

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Machine learning in catalysis journal April 2018
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Figures / Tables (5)

FIG. 1(p. 5)figure FIG. 1
in the legend refers to the orthorhombic unit cell. The background level, as measured without the SCO lm (but with the substrate), is shown by the gray-shaded area." data-ostiid="1560385">
FIG. 2(p. 6)figure FIG. 2
FIG. 3(p. 7)figure FIG. 3
FIG. 4(p. 8)figure FIG. 4
FIG. 5(p. 10)figure FIG. 5

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