Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen

In this work, we compare the CO oxidation performance of Pt single atom catalysts (SACs) prepared via two methods: (1) conventional wet chemical synthesis (strong electrostatic adsorption–SEA) with calcination at 350 °C in air; and (2) high temperature vapor phase synthesis (atom trapping–AT) with c...

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Bibliographic Details
Published in:Nature communications Vol. 10; no. 1; pp. 1358 - 10
Main Authors: Pereira-Hernández, Xavier Isidro, DeLaRiva, Andrew, Muravev, Valery, Kunwar, Deepak, Xiong, Haifeng, Sudduth, Berlin, Engelhard, Mark, Kovarik, Libor, Hensen, Emiel J. M., Wang, Yong, Datye, Abhaya K.
Format: Journal Article
Language:English
Published: London Nature Publishing Group UK 25.03.2019
Nature Publishing Group
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Subjects:
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140/146
140/58
147/137
639/638/77/884
639/638/77/885
639/638/77/887
Air temperature
Catalysis
Catalysts
Cerium oxides
Chemical synthesis
Cobalt
High temperature
Humanities and Social Sciences
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Low temperature
Metal particles
multidisciplinary
Organic chemistry
Oxidation
Oxygen
Photoelectron spectroscopy
Photoelectrons
Platinum
Pressure
Roasting
Science
Science (multidisciplinary)
Single atom catalysts
Temperature effects
Thermal stability
Vapor phases
Vapors
X ray photoelectron spectroscopy
ISSN:2041-1723, 2041-1723
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Summary:In this work, we compare the CO oxidation performance of Pt single atom catalysts (SACs) prepared via two methods: (1) conventional wet chemical synthesis (strong electrostatic adsorption–SEA) with calcination at 350 °C in air; and (2) high temperature vapor phase synthesis (atom trapping–AT) with calcination in air at 800 °C leading to ionic Pt being trapped on the CeO 2 in a thermally stable form. As-synthesized, both SACs are inactive for low temperature (<150 °C) CO oxidation. After treatment in CO at 275 °C, both catalysts show enhanced reactivity. Despite similar Pt metal particle size, the AT catalyst is significantly more active, with onset of CO oxidation near room temperature. A combination of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and CO temperature-programmed reduction (CO-TPR) shows that the high reactivity at low temperatures can be related to the improved reducibility of lattice oxygen on the CeO 2 support. While single-atom catalysts (SACs) have attracted a lot of interest, the nature of the active sites in SACs remains elusive. Here the authors elucidate that depositing single atoms via high temperature synthesis leads to improved reducibility of lattice oxygen on CeO2 yielding low temperature reactivity of Pt catalysts in CO oxidation.
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USDOE
AC05-76RL01830
PNNL-SA-132985
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-09308-5