Add time:08/03/2019 Source:sciencedirect.com
Although Ru3(CO)12 becomes a popular precursor for supported Ru catalysts nowadays, the activities of the catalysts prepared by thermolysis of the supported Ru3(CO)12 under different atmospheres have been rarely compared. We herein report the preparation of alumina-supported Ru samples by thermal activation of Ru3(CO)12 in air, H2 or N2, followed by activity test in the hydrogenation of 2-Benzylpyridine (cas 101-82-6) (BPy). When the supported Ru3(CO)12 was activated in air, RuO2 particles of 12–15 nm diameters were produced by complete oxidation of carbonyl groups. In contrast, thermal activation in H2 and N2 induced the formation of highly dispersed Ru0 particles of 1.4–2.3 nm diameters. In such activations methane was produced, suggesting that direct hydrogenation of CO coordinated to the Ru surface complex occurred in H2 while the coordinated CO reacted with ruthenium hydride species in N2. In the activity test for BPy hydrogenation, the samples prepared in H2 and N2 showed superior H2 storage efficiencies and higher rate constants compared to those prepared in air (reduced before the reaction). Additionally, the former samples were examined to be relatively stable even though exposed to ambient air for 7 days. Therefore, H2 and N2 gases are recommended for thermal activation of alumina-supported Ru3(CO)12.
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