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 |
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Pages (from-to) | 4044-4048 |
Number of pages | 5 |
Journal | ACS Catalysis |
Volume | 8 |
Issue number | 5 |
DOIs | |
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 |
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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