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Title: Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation

Abstract

While single-atom catalysts can provide high catalytic activity and selectivity, application in industrial catalysts demands long term performance and the ability to regenerate the catalysts. We have investigated the factors that lead to improved catalytic activity of a Pt/CeO2 catalyst for low temperature CO oxidation. Single-atom Pt/CeO2 becomes active for CO oxidation under lean condition only at elevated temperatures, because CO is strongly bound to ionic Pt sites. Reducing the catalyst, even under mild conditions, leads to onset of CO oxidation activity even at room temperature. This high activity state involves the transformation of mononuclear Pt species to sub-nanometer sized Pt particles. Under oxidizing conditions, the Pt can be restored to its stable, single-atom state. The key to facile regeneration is the ability to create mobile Pt species and suitable trapping sites on the support, making this a prototypical catalyst system for industrial application of single-atom catalysis.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1415696
Report Number(s):
PNNL-SA-126186
Journal ID: ISSN 0036-8075; 49339; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Science; Journal Volume: 358; Journal Issue: 6369
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Nie, Lei, Mei, Donghai, Xiong, Haifeng, Peng, Bo, Ren, Zhibo, Hernandez, Xavier Isidro Pereira, DeLaRiva, Andrew, Wang, Meng, Engelhard, Mark H., Kovarik, Libor, Datye, Abhaya K., and Wang, Yong. Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation. United States: N. p., 2017. Web. doi:10.1126/science.aao2109.
Nie, Lei, Mei, Donghai, Xiong, Haifeng, Peng, Bo, Ren, Zhibo, Hernandez, Xavier Isidro Pereira, DeLaRiva, Andrew, Wang, Meng, Engelhard, Mark H., Kovarik, Libor, Datye, Abhaya K., & Wang, Yong. Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation. United States. doi:10.1126/science.aao2109.
Nie, Lei, Mei, Donghai, Xiong, Haifeng, Peng, Bo, Ren, Zhibo, Hernandez, Xavier Isidro Pereira, DeLaRiva, Andrew, Wang, Meng, Engelhard, Mark H., Kovarik, Libor, Datye, Abhaya K., and Wang, Yong. Thu . "Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation". United States. doi:10.1126/science.aao2109.
@article{osti_1415696,
title = {Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation},
author = {Nie, Lei and Mei, Donghai and Xiong, Haifeng and Peng, Bo and Ren, Zhibo and Hernandez, Xavier Isidro Pereira and DeLaRiva, Andrew and Wang, Meng and Engelhard, Mark H. and Kovarik, Libor and Datye, Abhaya K. and Wang, Yong},
abstractNote = {While single-atom catalysts can provide high catalytic activity and selectivity, application in industrial catalysts demands long term performance and the ability to regenerate the catalysts. We have investigated the factors that lead to improved catalytic activity of a Pt/CeO2 catalyst for low temperature CO oxidation. Single-atom Pt/CeO2 becomes active for CO oxidation under lean condition only at elevated temperatures, because CO is strongly bound to ionic Pt sites. Reducing the catalyst, even under mild conditions, leads to onset of CO oxidation activity even at room temperature. This high activity state involves the transformation of mononuclear Pt species to sub-nanometer sized Pt particles. Under oxidizing conditions, the Pt can be restored to its stable, single-atom state. The key to facile regeneration is the ability to create mobile Pt species and suitable trapping sites on the support, making this a prototypical catalyst system for industrial application of single-atom catalysis.},
doi = {10.1126/science.aao2109},
journal = {Science},
number = 6369,
volume = 358,
place = {United States},
year = {Thu Dec 14 00:00:00 EST 2017},
month = {Thu Dec 14 00:00:00 EST 2017}
}