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Hidrogenolise de metilciclopentano sobre catalisadores de Ir-Au/[gama]-Al2O3

by Chimentão, Ricardo Jose

Abstract (Summary)
Ir/y-AhO3 and Ir-Au/y-AhO3 catalysts with total 8% ofweigth percentage were prepared by the incipient wetness method. The metaIs were added to the y-AhO3 in on step (co-impregnation) or in two steps (sucessive impregnation) as aqueous solutions of hexachloroiridic and tetrachloroauric acids. The percentage of Au atoms in the solids varied between 11 and 89. The catalysts were characterized by hydrogen chemisorption. The fraction of exposed Ir atoms in the solids prepared by co-impregnation and reduced at 600K increased between 0,63 and 0,67 as the amount of Au increased. For the catalysts prepared by sucessive impregnation the fraction of exposed Ir atoms variated between 0,65 and 0,3 as the amount of Au increased. The isosteric heat fo adsorption, calculated by the Clausius-Clapeyron equation, decreased linearly as coverage increase. For the solids prepared by coimpregnation and reduced at 600 K the isosteric heat of adsorption for the zero covered variated between 136,2 and 167,8 kJ/mol. For the solids prepared by impregnation sucessive the isosteric heat of adsorption for the zero covered variated between 104,5 e 151,9 kJ/mol. The methylcyclopentane hydrogenolysis reaction at 457 K on Ir/y-AhO3 and Ir-Au/y-AhO3 catalysts was studied and the turnover rate varied between 1,10xlO-2 /S-1 and 4,45 x 10-2/ S-I. The smal variation in turnover rate as the amount of Au increase suggests that there is an interaction between Au and Ir. In any event, the small change in the TOR confumed that this reaction is structure insensible. The linear Polanyi-type relation was assumed in the expression for the overall reaction rate. A correlation between the TOR and the H2 isosteric heat of adsorption was found for a surface 50 to 80% covered with H atoms. It was suggested that the surface was covered with both hydrogen and methylcyclopentane, and that hydrogen was present in the rate -determining step
This document abstract is also available in Portuguese.
Bibliographical Information:

Advisor:Gustavo Paim Valença; Gustavo Paim Valença [Orientador]; Gilberto Marques da Cruz; David dos Santos Cunha

School:Universidade Estadual de Campinas

School Location:Brazil

Source Type:Master's Thesis

Keywords:iridio hidrogenio catalisadores de metais transição

ISBN:

Date of Publication:07/18/2002

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