Journal
ACS APPLIED NANO MATERIALS
Volume 1, Issue 9, Pages 5258-5267Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.8b01256
Keywords
methane partial oxidation; ruthenium; nanocrystal; catalyst; syngas
Funding
- U.S. Department of Energy, Office of Sciences, Office of Basic Energy Sciences
- SUNCAT Center for Interfacial Science and Catalysis
- National Science Foundation Graduate Research Fellowship [DGE-1656518]
- School of Engineering at Stanford University
- Terman Faculty Fellowship
- National Science Foundation [ECCS-1542152]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
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The low-temperature conversion of methane into value-added products is an appealing goal due to the abundance of methane in the form of natural gas. Industrially, methane is used to produce synthesis gas (syngas), a precursor mixture used heavily in the production of ammonia, methanol, and synthetic fuels. In practice, this mixture is produced via the energy-intensive methane steam reforming reaction at temperatures between 750 and 1450 degrees C. The exothermic methane partial oxidation reaction stands as an alternative for syngas formation at lower temperatures, especially for gas to liquid fuels applications, yet awaits large-scale implementation due to dangerous operating conditions and temperatures. Using colloidally synthesized Ru catalysts, we identify two unifying rules that govern the low-temperature production of synthesis gas: depletion of oxygen within the catalyst bed and facile RuO2 -> Ru reduction kinetics, which is a strong function of supporting material and Ru nanostructure. Using these design rules, we demonstrate the enhanced low-temperature activity of a bifunctional Ru/Pd catalyst which produces synthesis gas at similar to 400 degrees C, with nearly complete CH4 conversion and CO selectivity at 670 degrees C.
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