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Interaction of hydrogen with supported Ru catalysts: High pressure in situ NMR studies

Journal Article · · Journal of Catalysis; (United States)
An in situ H nuclear magnetic resonance (NMR) technique has been employed to study the interaction of hydrogen with silica-supported ruthenium catalysts in the temperature range 300-473 K and at pressures of 10[sup [minus]5]-760 Torr. In addition to an upfield NMR peak (called [alpha]) occurring at [approximately] [minus]60 ppm and observed at low pressures (P < 100 Torr), the authors have noted the emergence of a second peak (called [beta]) occurring at [approximately] [minus]30 ppm at elevated pressures (P > 100 Torr). These two hydrogen populations represent adsorbed hydrogen interacting with Ru metal particles, as indicated by the observed Knight shifts. The [alpha] hydrogen species exists in the form of less mobile hydrogen species [alpha][sub 1], or a mobile hydrogen species [alpha][sub M] with heats of adsorption determined by microcalorimetry to be about 70 kJ/mol and 40 kJ/mol, respectively. The heat of adsorption of the [beta] species was determined to be approximately 10 kJ/mol. Hydrogen adsorption isotherms were obtained from the NMR peak intensities calibrated by a gadolinium-doped lanthanum hydride internal reference. A higher dispersion of metal particles correlated with a larger amount of the weakly adsorbed [beta] hydrogen species. The H/Ru[sub surface] ratio was observed to be in excess of 5 at elevated pressures (>500 Torr). The high H/Ru[sub surface] was due to the adsorption of large amounts of [beta] hydrogen. 53 refs., 9 figs., 1 tab.
DOE Contract Number:
W-7405-ENG-82
OSTI ID:
7275832
Journal Information:
Journal of Catalysis; (United States), Journal Name: Journal of Catalysis; (United States) Vol. 147:2; ISSN 0021-9517; ISSN JCTLA5
Country of Publication:
United States
Language:
English