Platinum-based heterogeneous catalysts are mostly used in various commercial chemical processes because of their high catalytic activity, influenced by the metal/oxide interaction. To design rational catalysts with high performance, it is crucial to understand the relationship between the metal–oxide interface and the reaction pathway. Here, we investigate the role of oxygen defect sites in the reaction mechanism for CO oxidation using Pt nanoparticles supported on mesoporous TiO2 catalysts with oxygen defects. We show an intrinsic correlation between the catalytic reactivity and the local properties of titania with oxygen defects (i.e., Ti3+ sites). In situ infrared spectroscopy observations of the Pt/mesoporous TiO2−x catalyst indicate that an oxygen molecule bond can be activated at the perimeter between the Pt and an oxygen vacancy in TiO2 by neighboring CO molecules on the Pt surface before CO oxidation begins. The proposed reaction pathways for O2 activation at the Pt/TiO2−x interface based on density functional theory confirm our experimental findings. We suggest that this provides valuable insight into the intrinsic origin of the metal/support interaction influenced by the presence of oxygen vacancies, which clarifies the pivotal role played by the support.
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Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO2 during CO oxidation
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21 December 2019
Research Article|
December 19 2019
Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO2 during CO oxidation
Sunyoung Oh;
Sunyoung Oh
a)
1
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)
, Daejeon 34141, South Korea
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
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Hyunwoo Ha
;
Hyunwoo Ha
a)
3
Department of Materials Science and Engineering, Chungnam National University
, Daejeon 34134, South Korea
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Hanseul Choi;
Hanseul Choi
1
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)
, Daejeon 34141, South Korea
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
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Changbum Jo;
Changbum Jo
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
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Jangkeun Cho;
Jangkeun Cho
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
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Hyuk Choi;
Hyuk Choi
3
Department of Materials Science and Engineering, Chungnam National University
, Daejeon 34134, South Korea
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Ryong Ryoo;
Ryong Ryoo
b)
1
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)
, Daejeon 34141, South Korea
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
b)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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Hyun You Kim;
Hyun You Kim
b)
3
Department of Materials Science and Engineering, Chungnam National University
, Daejeon 34134, South Korea
b)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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Jeong Young Park
Jeong Young Park
b)
1
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)
, Daejeon 34141, South Korea
2
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
, Daejeon 34141, South Korea
b)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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a)
Contributions: S. Oh and H. Ha contributed equally to this work.
b)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
Note: This article is part of the JCP Special Topic on Oxide Chemistry and Catalysis.
J. Chem. Phys. 151, 234716 (2019)
Article history
Received:
October 12 2019
Accepted:
November 26 2019
Citation
Sunyoung Oh, Hyunwoo Ha, Hanseul Choi, Changbum Jo, Jangkeun Cho, Hyuk Choi, Ryong Ryoo, Hyun You Kim, Jeong Young Park; Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO2 during CO oxidation. J. Chem. Phys. 21 December 2019; 151 (23): 234716. https://doi.org/10.1063/1.5131464
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