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Title: Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation

Abstract

Ceria-supported Pd is a promising heterogeneous catalyst for CO oxidation relevant to environmental cleanup reactions. Pd loaded onto a nanorod form of ceria exposing predominantly (111) facets is already active at 50 °C. Here we report a combination of CO-FTIR spectroscopy and theoretical calculations that allows assigning different forms of Pd on the CeO2(111) surface during reaction conditions. Single Pd atoms stabilized in the form of PdO and PdO2 in a CO/O2 atmosphere participate in a catalytic cycle involving very low activation barriers for CO oxidation. In conclusion, the presence of single Pd atoms on the Pd/CeO2-nanorod, corroborated by aberration-corrected TEM and CO-FTIR spectroscopy, is considered pivotal to its high CO oxidation activity.

Authors:
 [1];  [1]; ORCiD logo [1];  [2];  [2];  [2];  [2]; ORCiD logo [1]
  1. Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
  2. Univ. of New Mexico, Albuquerque, NM (United States)
Publication Date:
Research Org.:
The Netherlands Organization for Scientific Research (NWO) (The Netherlands); Univ. of New Mexico, Albuquerque, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1414915
Alternate Identifier(s):
OSTI ID: 1508266
Grant/Contract Number:  
FG02-05ER15712
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cerium oxide; CO oxidation; computational modeling; FTIR; mechanism; palladium; single site

Citation Formats

Spezzati, Giulia, Su, Yaqiong, Hofmann, Jan P., Benavidez, Angelica D., DeLaRiva, Andrew T., McCabe, Jay, Datye, Abhaya K., and Hensen, Emiel J. M. Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation. United States: N. p., 2017. Web. doi:10.1021/acscatal.7b02001.
Spezzati, Giulia, Su, Yaqiong, Hofmann, Jan P., Benavidez, Angelica D., DeLaRiva, Andrew T., McCabe, Jay, Datye, Abhaya K., & Hensen, Emiel J. M. Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation. United States. doi:10.1021/acscatal.7b02001.
Spezzati, Giulia, Su, Yaqiong, Hofmann, Jan P., Benavidez, Angelica D., DeLaRiva, Andrew T., McCabe, Jay, Datye, Abhaya K., and Hensen, Emiel J. M. Thu . "Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation". United States. doi:10.1021/acscatal.7b02001. https://www.osti.gov/servlets/purl/1414915.
@article{osti_1414915,
title = {Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation},
author = {Spezzati, Giulia and Su, Yaqiong and Hofmann, Jan P. and Benavidez, Angelica D. and DeLaRiva, Andrew T. and McCabe, Jay and Datye, Abhaya K. and Hensen, Emiel J. M.},
abstractNote = {Ceria-supported Pd is a promising heterogeneous catalyst for CO oxidation relevant to environmental cleanup reactions. Pd loaded onto a nanorod form of ceria exposing predominantly (111) facets is already active at 50 °C. Here we report a combination of CO-FTIR spectroscopy and theoretical calculations that allows assigning different forms of Pd on the CeO2(111) surface during reaction conditions. Single Pd atoms stabilized in the form of PdO and PdO2 in a CO/O2 atmosphere participate in a catalytic cycle involving very low activation barriers for CO oxidation. In conclusion, the presence of single Pd atoms on the Pd/CeO2-nanorod, corroborated by aberration-corrected TEM and CO-FTIR spectroscopy, is considered pivotal to its high CO oxidation activity.},
doi = {10.1021/acscatal.7b02001},
journal = {ACS Catalysis},
number = 10,
volume = 7,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 33 works
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Figures / Tables:

Figure 1 Figure 1: (a) CO oxidation on (black) CeO2-rods and (red) Pd/ CeO2-rod, (b) AC-TEM image of CeO2 nanorods showing exposed (111) facets, (c) AC-TEM image of Pd/CeO2-rod after air calcination at 300 °C showing the absence of particles, and (d) AC-TEM image of the Pd/CeO2-rod sample after reduction at 300more » °C showing a well-defined metallic Pd nanoparticle.« less

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Works referencing / citing this record:

Thermally Induced Structural Evolution of Palladium‐Ceria Catalysts. Implication for CO Oxidation
journal, June 2019

  • Stonkus, Olga A.; Kardash, Tatyana Yu.; Slavinskaya, Elena M.
  • ChemCatChem, Vol. 11, Issue 15
  • DOI: 10.1002/cctc.201900752

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
journal, July 2019

  • Li, Xuning; Yang, Xiaofeng; Huang, Yanqiang
  • Advanced Materials, Vol. 31, Issue 50
  • DOI: 10.1002/adma.201902031

Towards dense single-atom catalysts for future automotive applications
journal, July 2019


Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
journal, July 2019

  • Li, Xuning; Yang, Xiaofeng; Huang, Yanqiang
  • Advanced Materials, Vol. 31, Issue 50
  • DOI: 10.1002/adma.201902031

Thermally Induced Structural Evolution of Palladium‐Ceria Catalysts. Implication for CO Oxidation
journal, June 2019

  • Stonkus, Olga A.; Kardash, Tatyana Yu.; Slavinskaya, Elena M.
  • ChemCatChem, Vol. 11, Issue 15
  • DOI: 10.1002/cctc.201900752

Towards dense single-atom catalysts for future automotive applications
journal, July 2019


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.