Journal
ACS CATALYSIS
Volume 8, Issue 5, Pages 4044-4048Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b00004
Keywords
single-atom catalysts; direct methane conversion; platinum; ceria nanocrystals; carbon coking
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Funding
- IDEAS Program of the Advanced Research Projects Agency-Energy (ARPA-E), Department of Energy (DOE)
- Johns Hopkins Catalyst Award
- National Science Foundation's Energy Resarch Center for Strategic Transformation of Alkane Resources (CISTAR) [EEC-1647722]
- U.S. Department of Energy (DOE), Office of Basic Energy Science [DE-SC0012704]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Department of Energy
- MRCAT
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Nanoceria-supported atomic Pt catalysts (denoted as Pt-1@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 degrees 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 Pt-1@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 C-2 products (ethane, ethylene, and acetylene). Comparative studies of the Pt-1@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 C-2 hydrocarbons.
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