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Title: Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts

Abstract

Although perovskites have been widely used in catalysis, tuning their surface terminations to control reaction selectivities has not been well established. In this work, we employ multiple surface sensitive techniques to characterize the surface termination (one aspect of surface reconstruction) of SrTiO3 (STO) after thermal pretreatment (Sr-enrichment) and chemical etching (Ti-enrichment). We show, using the conversion of 2-propanol as a probe reaction, that the surface termination of STO can be controlled to greatly tune catalytic acid/base properties and consequently the reaction selectivities in a wide range, which are inaccessible using single metal oxides, either SrO or TiO2. Density functional theory (DFT) calculations well explain the selectivity tuning and reaction mechanism on different surface terminations of STO. Similar catalytic tunability is also observed on BaZrO3, highlighting the generality of the finding from this work.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [3];  [1];  [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of California, Riverside, CA (United States)
  3. Tennessee Technological Univ., Cookeville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1399923
Alternate Identifier(s):
OSTI ID: 1378301
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 33; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Polo-Garzon, Felipe, Yang, Shi-Ze, Fung, Victor, Foo, Guo Shiou, Bickel, Elizabeth E., Chisholm, Matthew F., Jiang, De-en, and Wu, Zili. Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts. United States: N. p., 2017. Web. https://doi.org/10.1002/anie.201704656.
Polo-Garzon, Felipe, Yang, Shi-Ze, Fung, Victor, Foo, Guo Shiou, Bickel, Elizabeth E., Chisholm, Matthew F., Jiang, De-en, & Wu, Zili. Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts. United States. https://doi.org/10.1002/anie.201704656
Polo-Garzon, Felipe, Yang, Shi-Ze, Fung, Victor, Foo, Guo Shiou, Bickel, Elizabeth E., Chisholm, Matthew F., Jiang, De-en, and Wu, Zili. Wed . "Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts". United States. https://doi.org/10.1002/anie.201704656. https://www.osti.gov/servlets/purl/1399923.
@article{osti_1399923,
title = {Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts},
author = {Polo-Garzon, Felipe and Yang, Shi-Ze and Fung, Victor and Foo, Guo Shiou and Bickel, Elizabeth E. and Chisholm, Matthew F. and Jiang, De-en and Wu, Zili},
abstractNote = {Although perovskites have been widely used in catalysis, tuning their surface terminations to control reaction selectivities has not been well established. In this work, we employ multiple surface sensitive techniques to characterize the surface termination (one aspect of surface reconstruction) of SrTiO3 (STO) after thermal pretreatment (Sr-enrichment) and chemical etching (Ti-enrichment). We show, using the conversion of 2-propanol as a probe reaction, that the surface termination of STO can be controlled to greatly tune catalytic acid/base properties and consequently the reaction selectivities in a wide range, which are inaccessible using single metal oxides, either SrO or TiO2. Density functional theory (DFT) calculations well explain the selectivity tuning and reaction mechanism on different surface terminations of STO. Similar catalytic tunability is also observed on BaZrO3, highlighting the generality of the finding from this work.},
doi = {10.1002/anie.201704656},
journal = {Angewandte Chemie (International Edition)},
number = 33,
volume = 56,
place = {United States},
year = {2017},
month = {7}
}

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Cited by: 8 works
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