期刊
NATURE CATALYSIS
卷 4, 期 10, 页码 882-891出版社
NATURE PORTFOLIO
DOI: 10.1038/s41929-021-00686-y
关键词
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资金
- Herbert L. Stiles Professorship
- Iowa State University College of Engineering
- National Science Foundation [EEC-1647722]
- R. Games Slayter Fund of Purdue University
- Varma Reaction Engineering Research Fund of Purdue University
- NSF-CBET Award [1804712]
- University of Michigan College of Engineering
- US Department of Energy, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- US Department of Energy [DE-AC02-07CH11358]
The study demonstrates that atomically thin Pt nanolayers supported on MXene can efficiently catalyze the conversion of methane to ethane/ethylene, operating for 72 hours at high temperatures with >98% selectivity, providing important insights into designing highly active and stable catalysts.
Efficient and direct conversion of methane to value-added products has been a long-term challenge in shale gas applications. Here, we show that atomically thin nanolayers of Pt with a single or double atomic layer thickness, supported on a two-dimensional molybdenum titanium carbide (MXene), catalyse non-oxidative coupling of methane to ethane/ethylene (C-2). Kinetic and theoretical studies, combined with in-situ spectroscopic and microscopic characterizations, demonstrate that Pt nanolayers anchored at the hexagonal close-packed sites of the MXene support can activate the first C-H bond of methane to form methyl radicals that favour desorption over further dehydrogenation and thus suppress coke deposition. At 750 degrees C and 7% methane conversion, the catalyst runs for 72 hours of continuous operation without deactivation and exhibits >98% selectivity towards C-2 products, with a turnover frequency of 0.2-0.6 s(-1). Our findings provide insights into the design of highly active and stable catalysts for methane activation and create a platform for developing atomically thin supported metal catalysts.
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