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

Xavier Isidro Pereira-Hernández; Andrew DeLaRiva; Valery Muravev; Deepak Kunwar; Haifeng Xiong; Berlin Sudduth; Mark Engelhard; Libor Kovarik; Emiel J.M. Hensen; Yong Wang; Abhaya K. Datye

doi:10.1038/s41467-019-09308-5

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

Xavier Isidro Pereira-Hernández
, Andrew DeLaRiva
, Valery Muravev
, Deepak Kunwar
, Haifeng Xiong
, Berlin Sudduth
, Mark Engelhard
, Libor Kovarik
, Emiel J.M. Hensen (Corresponding author)
, Yong Wang (Corresponding author)
, Abhaya K. Datye (Corresponding author)

Research output: Contribution to journal › Article › Academic › peer-review

423 Citations (Scopus)

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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.

Original language	English
Article number	1358
Number of pages	10
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-09308-5
Publication status	Published - 25 Mar 2019

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Pereira-Hernández, X. I., DeLaRiva, A., Muravev, V., Kunwar, D., Xiong, H., Sudduth, B., Engelhard, M., Kovarik, L., Hensen, E. J. M., Wang, Y., & Datye, A. K. (2019). Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen. Nature Communications, 10(1), Article 1358. https://doi.org/10.1038/s41467-019-09308-5

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title = "Tuning Pt-CeO2 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. ",

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AU - Pereira-Hernández, Xavier Isidro

AU - DeLaRiva, Andrew

AU - Muravev, Valery

AU - Kunwar, Deepak

AU - Xiong, Haifeng

AU - Sudduth, Berlin

AU - Engelhard, Mark

AU - Kovarik, Libor

AU - Hensen, Emiel J.M.

AU - Wang, Yong

AU - Datye, Abhaya K.

PY - 2019/3/25

Y1 - 2019/3/25

N2 - 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.

AB - 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.

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VL - 10

JO - Nature Communications

JF - Nature Communications

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

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

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Catalyst advance removes pollutants at low temperatures

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