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Hydrocarbon conversions with some intermetallic catalysts

Hydrocarbon conversions with some intermetallic catalysts

Authors :
J. M. Brown
John M. Winterbottom
A. Bahia
I. T. Caga
I. R. Harris
C. E. King
Source :
Journal of Chemical Technology & Biotechnology. 48:351-360
Publication Year :
2007
Publisher :
Wiley, 2007.

Abstract

The intermetallic pseudo-binary alloys of the general type ZrRh3-xPdx and ZrRh3-xRux (0 < × < 3) have been prepared by argon arc melting and melt quenching of the constituent elements. The alloys were powdered and employed as catalysts for (i) hydrogenation of oct-1-yne in the liquid phase at 101.32 kPa total pressure and 70°C, (ii) hydrogenation of buta-1,3-diene in the gas phase at 101.32 kPa total pressure in the temperature range 45–225°C, and (iii) hydrogenolysis of n-pentane in the gas phase at 101.32 kPa total pressure and in the temperature range 200–400°C. Activity and selectivity measurements were made with respect to (i) alkene formation for the hydrogenation reactions, and (ii) C2 + C3-alkane formation for the hydrogenolysis reaction. The activity of the alloy series appears to correlate to some degree with the electronic properties and hydrogen sorption capacity of the intermetallic alloys. Auger electron spectroscopy measurements revealed that for ZrRh3-xPdx alloys both the surface and bulk compositions were in good agreement; this behaviour is contrasted briefly with that of CeRh3-xPdx alloys which, unlike ZrRh3-x alloys, suffered significant oxygen interaction in the surface and sub-surface layers, although this did not affect Rh:Pd ratios. Catalysts that were active for hydrogenation were inactive for hydrogenolysis and vice versa. However, selectivity values for the hydrogenation reactions generally reflected the behaviour of the predominant noble transition metal. Again, the behaviour of ZrRh3-xPdx and CeRh3-x alloys is contrasted, since the latter were more selective for butene formation from buta-1,3-diene, and attributed to the oxygen Contamination of the surface. Further more, the selectivity of both ZrPd and CePd, for 1-octyne and butu-l j-dene hydrogenation was significantly greater than that of palladium by virtue of the fact that the intermetallics were found to be largely inactive for alkene hydrogenation.

Details

ISSN :
10974660 and 02682575
Volume :
48
Database :
OpenAIRE
Journal :
Journal of Chemical Technology & Biotechnology
Accession number :
edsair.doi...........758a83f905e62a183b65fe007b8909c1
Full Text :
https://doi.org/10.1002/jctb.280480310