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Title: Tuning Pt-CeO 2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen

Abstract

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.

Authors:
ORCiD logo [1];  [2];  [3];  [2]; ORCiD logo [2];  [1]; ORCiD logo [4];  [4]; ORCiD logo [3];  [5]; ORCiD logo [2]
  1. Washington State Univ., Pullman, WA (United States)
  2. Univ. of New Mexico, Albuquerque, NM (United States)
  3. Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1507543
Report Number(s):
PNNL-SA-132985
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Pereira-Hernández, Xavier Isidro, DeLaRiva, Andrew, Muravev, Valery, Kunwar, Deepak, Xiong, Haifeng, Sudduth, Berlin, Engelhard, Mark, Kovarik, Libor, Hensen, Emiel J. M., Wang, Yong, and Datye, Abhaya K.. Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen. United States: N. p., 2019. Web. doi:10.1038/S41467-019-09308-5.
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.. Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen. United States. doi:10.1038/S41467-019-09308-5.
Pereira-Hernández, Xavier Isidro, DeLaRiva, Andrew, Muravev, Valery, Kunwar, Deepak, Xiong, Haifeng, Sudduth, Berlin, Engelhard, Mark, Kovarik, Libor, Hensen, Emiel J. M., Wang, Yong, and Datye, Abhaya K.. Mon . "Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen". United States. doi:10.1038/S41467-019-09308-5. https://www.osti.gov/servlets/purl/1507543.
@article{osti_1507543,
title = {Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen},
author = {Pereira-Hernández, Xavier Isidro and DeLaRiva, Andrew and Muravev, Valery and Kunwar, Deepak and Xiong, Haifeng and Sudduth, Berlin and Engelhard, Mark and Kovarik, Libor and Hensen, Emiel J. M. and Wang, Yong and Datye, Abhaya K.},
abstractNote = {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 CeO2 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 CeO2 support.},
doi = {10.1038/S41467-019-09308-5},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {3}
}

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