TY - JOUR
T1 - Atomic level fluxional behavior and activity of CeO2-supported Pt catalysts for CO oxidation
AU - Vincent, Joshua L.
AU - Crozier, Peter A.
N1 - Funding Information:
The authors gratefully acknowledge funding for this research from NSF grant CBET 1604971. The authors thank Arizona State University’s John M. Cowley Center for High Resolution Electron Microscopy for microscope access and use. The authors also gratefully acknowledge the use of environmental electron microscopy facilities at the National Institute of Standards and Technology in Gaithersburg, MD, and in particular would like to acknowledge the helpfulness and hospitality of Dr. Wei-Chang David Yang, Dr. Canhui Wang, and Dr. Renu Sharma. Additionally, the authors are grateful to Mr. Piyush Haluai for assistance with measuring the strain of Ce atomic columns.
Publisher Copyright:
© 2021, The Author(s).
PY - 2021/12/1
Y1 - 2021/12/1
N2 - Reducible oxides are widely used catalyst supports that can increase oxidation reaction rates by transferring lattice oxygen at the metal-support interface. There are many outstanding questions regarding the atomic-scale dynamic meta-stability (i.e., fluxional behavior) of the interface during catalysis. Here, we employ aberration-corrected operando electron microscopy to visualize the structural dynamics occurring at and near Pt/CeO2 interfaces during CO oxidation. We show that the catalytic turnover frequency correlates with fluxional behavior that (a) destabilizes the supported Pt particle, (b) marks an enhanced rate of oxygen vacancy creation and annihilation, and (c) leads to increased strain and reduction in the CeO2 support surface. Overall, the results implicate the interfacial Pt-O-Ce bonds anchoring the Pt to the support as being involved also in the catalytically-driven oxygen transfer process, and they suggest that oxygen reduction takes place on the highly reduced CeO2 surface before migrating to the interfacial perimeter for reaction with CO.
AB - Reducible oxides are widely used catalyst supports that can increase oxidation reaction rates by transferring lattice oxygen at the metal-support interface. There are many outstanding questions regarding the atomic-scale dynamic meta-stability (i.e., fluxional behavior) of the interface during catalysis. Here, we employ aberration-corrected operando electron microscopy to visualize the structural dynamics occurring at and near Pt/CeO2 interfaces during CO oxidation. We show that the catalytic turnover frequency correlates with fluxional behavior that (a) destabilizes the supported Pt particle, (b) marks an enhanced rate of oxygen vacancy creation and annihilation, and (c) leads to increased strain and reduction in the CeO2 support surface. Overall, the results implicate the interfacial Pt-O-Ce bonds anchoring the Pt to the support as being involved also in the catalytically-driven oxygen transfer process, and they suggest that oxygen reduction takes place on the highly reduced CeO2 surface before migrating to the interfacial perimeter for reaction with CO.
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U2 - 10.1038/s41467-021-26047-8
DO - 10.1038/s41467-021-26047-8
M3 - Article
C2 - 34608153
AN - SCOPUS:85116351477
SN - 2041-1723
VL - 12
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 5789
ER -