Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

Deepak Kunwar; Shulan Zhou; Andrew Delariva; Eric J. Peterson; Haifeng Xiong; Xavier Isidro Pereira-Hernández; Stephen C. Purdy; Rik Ter Veen; Hidde H. Brongersma; Jeffrey T. Miller; Hiroki Hashiguchi; Libor Kovarik; Sen Lin; Hua Guo; Yong Wang; Abhaya K. Datye

doi:10.1021/acscatal.8b04885

Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

Deepak Kunwar, Shulan Zhou, Andrew Delariva, Eric J. Peterson, Haifeng Xiong, Xavier Isidro Pereira-Hernández, Stephen C. Purdy, Rik Ter Veen, Hidde H. Brongersma, Jeffrey T. Miller, Hiroki Hashiguchi, Libor Kovarik, Sen Lin, Hua Guo, Yong Wang, Abhaya K. Datye

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

247 Scopus citations

Abstract

Single-atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt % Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO ₂ with under-coordinated cerium cations present at CeO ₂ (111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single-atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter resistance of ceria-supported metal catalysts.

Original language	English
Pages (from-to)	3978-3990
Number of pages	13
Journal	ACS Catalysis
Volume	9
Issue number	5
DOIs	https://doi.org/10.1021/acscatal.8b04885
State	Published - May 3 2019
Externally published	Yes

Funding

The research was supported by the US Department of Energy (DOE) grant DE-FG02-05ER15712. Additional funding was provided from US National Science Foundation grants EEC-1647722 (CISTAR), the National Natural Science Foundation of China grant 21673040, and the US Air Force Office of Scientific Research grants FA9550-15-1-0305 and FA9550-18-1-0413. XIPH thanks Fulbright Colombia and Colciencias, SZ thanks the China Scholarship Council (201608360178). The research utilized the Advanced Photon Source supported by the U.S. DOE under contract No. DE-AC02-06CH11357 and the Environmental Molecular Sciences Laboratory located at Pacific Northwest National Laboratory, supported by the U.S. DOE Office of Biological and Environmental Research. MRCAT operations and beamline 10-ID are supported by the DOE and the MRCAT member institutions.

Funders	Funder number
CISTAR
Fulbright Colombia and Colciencias
U.S. DOE	DE-AC02-06CH11357
U.S. DOE Office of Biological and Environmental Research
US Department of Energy
National Science Foundation	EEC-1647722
U.S. Department of Energy	DE-FG02-05ER15712
Air Force Office of Scientific Research	FA9550-18-1-0413, FA9550-15-1-0305
National Natural Science Foundation of China	21673040
China Scholarship Council	201608360178

Keywords

atom trapping
catalyst preparation
ionic Pt
single-atom catalysis
thermal stability

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10.1021/acscatal.8b04885

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Kunwar, D., Zhou, S., Delariva, A., Peterson, E. J., Xiong, H., Pereira-Hernández, X. I., Purdy, S. C., Ter Veen, R., Brongersma, H. H., Miller, J. T., Hashiguchi, H., Kovarik, L., Lin, S., Guo, H., Wang, Y., & Datye, A. K. (2019). Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support. ACS Catalysis, 9(5), 3978-3990. https://doi.org/10.1021/acscatal.8b04885

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title = "Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support",

abstract = " Single-atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt % Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO 2 with under-coordinated cerium cations present at CeO 2 (111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single-atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter resistance of ceria-supported metal catalysts.",

keywords = "atom trapping, catalyst preparation, ionic Pt, single-atom catalysis, thermal stability",

author = "Deepak Kunwar and Shulan Zhou and Andrew Delariva and Peterson, {Eric J.} and Haifeng Xiong and Pereira-Hern{\'a}ndez, {Xavier Isidro} and Purdy, {Stephen C.} and {Ter Veen}, Rik and Brongersma, {Hidde H.} and Miller, {Jeffrey T.} and Hiroki Hashiguchi and Libor Kovarik and Sen Lin and Hua Guo and Yong Wang and Datye, {Abhaya K.}",

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doi = "10.1021/acscatal.8b04885",

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Kunwar, D, Zhou, S, Delariva, A, Peterson, EJ, Xiong, H, Pereira-Hernández, XI, Purdy, SC, Ter Veen, R, Brongersma, HH, Miller, JT, Hashiguchi, H, Kovarik, L, Lin, S, Guo, H, Wang, Y & Datye, AK 2019, 'Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support', ACS Catalysis, vol. 9, no. 5, pp. 3978-3990. https://doi.org/10.1021/acscatal.8b04885

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T1 - Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

AU - Kunwar, Deepak

AU - Zhou, Shulan

AU - Delariva, Andrew

AU - Peterson, Eric J.

AU - Xiong, Haifeng

AU - Pereira-Hernández, Xavier Isidro

AU - Purdy, Stephen C.

AU - Ter Veen, Rik

AU - Brongersma, Hidde H.

AU - Miller, Jeffrey T.

AU - Hashiguchi, Hiroki

AU - Kovarik, Libor

AU - Lin, Sen

AU - Guo, Hua

AU - Wang, Yong

AU - Datye, Abhaya K.

PY - 2019/5/3

Y1 - 2019/5/3

N2 - Single-atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt % Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO 2 with under-coordinated cerium cations present at CeO 2 (111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single-atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter resistance of ceria-supported metal catalysts.

AB - Single-atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt % Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO 2 with under-coordinated cerium cations present at CeO 2 (111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single-atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter resistance of ceria-supported metal catalysts.

KW - atom trapping

KW - catalyst preparation

KW - ionic Pt

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KW - thermal stability

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Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

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