Nanoceria-Supported Single-Atom Platinum Catalysts for Direct Methane Conversion

Pengfei Xie; Tiancheng Pu; Anmin Nie; Sooyeon Hwang; Stephen C. Purdy; Wenjian Yu; Dong Su; Jeffrey T. Miller; Chao Wang

doi:10.1021/acscatal.8b00004

Nanoceria-Supported Single-Atom Platinum Catalysts for Direct Methane Conversion

Pengfei Xie, Tiancheng Pu, Anmin Nie, Sooyeon Hwang, Stephen C. Purdy, Wenjian Yu, Dong Su, Jeffrey T. Miller, Chao Wang

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

228 Scopus citations

Abstract

Nanoceria-supported atomic Pt catalysts (denoted as Pt₁@CeO₂) have been synthesized and demonstrated with advanced catalytic performance for the nonoxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1000 °C), with the atomic dispersion of Pt characterized by combining aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt₁@CeO₂ catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C and 74.6% selectivity toward C₂ products (ethane, ethylene, and acetylene). Comparative studies of the Pt₁@CeO₂ catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C₂ hydrocarbons.

Original language	English
Pages (from-to)	4044-4048
Number of pages	5
Journal	ACS Catalysis
Volume	8
Issue number	5
DOIs	https://doi.org/10.1021/acscatal.8b00004
State	Published - May 4 2018
Externally published	Yes

Funding

This work was supported by the IDEAS Program of the Advanced Research Projects Agency−Energy (ARPA-E), Department of Energy (DOE), and the Johns Hopkins Catalyst Award. Partial funding for S.C.P. and J.T.M. was provided as part of the National Science Foundation’s Energy Resarch Center for Strategic Transformation of Alkane Resources (CISTAR) under Cooperative Agreement No. EEC-1647722. Electron microscopy work was performed at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy (DOE), Office of Basic Energy Science, under contract DE-SC0012704. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract No. DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions.

Funders	Funder number
CISTAR
IDEAS Program of the Advanced Research Projects Agency−Energy
Johns Hopkins Catalyst Award
National Science Foundation’s Energy Resarch Center for Strategic Transformation of Alkane Resources
Office of Basic Energy Science	DE-SC0012704
Office of Basic Energy Sciences
National Science Foundation	1647722
U.S. Department of Energy
Advanced Research Projects Agency - Energy
Brookhaven National Laboratory
Institute for Functional Nanomaterials

Keywords

carbon coking
ceria nanocrystals
direct methane conversion
platinum
single-atom catalysts

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10.1021/acscatal.8b00004

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title = "Nanoceria-Supported Single-Atom Platinum Catalysts for Direct Methane Conversion",

abstract = "Nanoceria-supported atomic Pt catalysts (denoted as Pt1@CeO2) have been synthesized and demonstrated with advanced catalytic performance for the nonoxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1000 °C), with the atomic dispersion of Pt characterized by combining aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt1@CeO2 catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C and 74.6% selectivity toward C2 products (ethane, ethylene, and acetylene). Comparative studies of the Pt1@CeO2 catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C2 hydrocarbons.",

keywords = "carbon coking, ceria nanocrystals, direct methane conversion, platinum, single-atom catalysts",

author = "Pengfei Xie and Tiancheng Pu and Anmin Nie and Sooyeon Hwang and Purdy, {Stephen C.} and Wenjian Yu and Dong Su and Miller, {Jeffrey T.} and Chao Wang",

note = "Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

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AU - Xie, Pengfei

AU - Pu, Tiancheng

AU - Nie, Anmin

AU - Hwang, Sooyeon

AU - Purdy, Stephen C.

AU - Yu, Wenjian

AU - Su, Dong

AU - Miller, Jeffrey T.

AU - Wang, Chao

PY - 2018/5/4

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N2 - Nanoceria-supported atomic Pt catalysts (denoted as Pt1@CeO2) have been synthesized and demonstrated with advanced catalytic performance for the nonoxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1000 °C), with the atomic dispersion of Pt characterized by combining aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt1@CeO2 catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C and 74.6% selectivity toward C2 products (ethane, ethylene, and acetylene). Comparative studies of the Pt1@CeO2 catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C2 hydrocarbons.

AB - Nanoceria-supported atomic Pt catalysts (denoted as Pt1@CeO2) have been synthesized and demonstrated with advanced catalytic performance for the nonoxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1000 °C), with the atomic dispersion of Pt characterized by combining aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt1@CeO2 catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C and 74.6% selectivity toward C2 products (ethane, ethylene, and acetylene). Comparative studies of the Pt1@CeO2 catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C2 hydrocarbons.

KW - carbon coking

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KW - single-atom catalysts

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Nanoceria-Supported Single-Atom Platinum Catalysts for Direct Methane Conversion

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