Isotopic equilibration reaction of dinitrogen over Raney ruthenium: Importance of the structural factor

Journal Article · Mon Aug 01 04:00:00 EDT 1988 · Journal of Catalysis; (USA)

DOI:https://doi.org/10.1016/0021-9517(88)90162-5· OSTI ID:6551961

Ogata, Yoichi; Aika, Kenichi; Onishi, Takaharu ^[1]

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1. Tokyo Institute of Technology, Yokohama (Japan)

The isotopic equilibration reaction of dinitrogen ({sup 28}N{sub 2} + {sup 30}N{sub 2} = 2{sup 29}N{sub 2}) was studied over three Ru catalysts: stabilized Raney Ru, Al-Ru alloy, and Ru powder. The turnover frequency (TOF) at 588 K ranges from 10{sup {minus}6} to 10{sup {minus}2} and depends on the Al/Ru ratio and the microcrystal size of Ru. The highest TOFs are obtained over samples leached at 373 K from alloys having an atomic percent of Ru from 6 to 33. These samples have a smaller average Ru crystal size and a lower Al content, ranging from 8 to 18 mol% as measured by X-ray photoelectron spectroscopy (XPS). The authors also suggest that the high activity is related to strongly adsorbed nitrogen, the uptake of which exceeds hydrogen adsorption. Almost no XPS chemical shift is observed for any leached Raney Ru, whereas the Ru 3d binding energy in Al-Ru alloys is about 1 eV lower than that in Ru metal powder. In spite of the pronounced chemical shift, the TOF on Al-Ru alloy is quite low. Results suggest that structural factors are mot important in this system, rather than the electronic factor that has been emphasized for supported Ru catalysts.

• OSTI ID: 6551961
• Journal Information: Journal of Catalysis; (USA), Journal Name: Journal of Catalysis; (USA) Vol. 112:2; ISSN 0021-9517; ISSN JCTLA
• Country of Publication: United States
• Language: English

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ALUMINIUM
AMMONIA
BIMETALS
CATALYSTS
CATALYTIC EFFECTS
CHEMICAL ANALYSIS
CHEMICAL SHIFT
COHERENT SCATTERING
COMPARATIVE EVALUATIONS
CRYSTAL STRUCTURE
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ELECTRON MICROPROBE ANALYSIS
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HYDRIDES
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HYDROGEN COMPOUNDS
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METALS
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MICROSCOPY
MICROSTRUCTURE
NITROGEN
NITROGEN COMPOUNDS
NITROGEN HYDRIDES
NONMETALS
PHOTOELECTRON SPECTROSCOPY
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RUTHENIUM
SCANNING ELECTRON MICROSCOPY
SCATTERING
SORPTION
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TRANSITION ELEMENTS
TRANSMISSION ELECTRON MICROSCOPY
X-RAY DIFFRACTION
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