Highly active Ru/TiO2 nanostructures for total catalytic oxidation of propane

Abstract

Ruthenium is a robust catalyst for a variety of applications in environmental heterogeneous catalysis. The catalytic performance of Ru/TiO2 materials, synthesized by using the deposition precipitation with urea method, was assessed in the catalytic oxidation of C3H8, varying the ruthenium loading. The highest catalytic reactivity was obtained for a Ru loading of 2 wt. % in comparison with the 1, 1.5, 3, and 4 wt. % Ru catalysts. The physicochemical properties of the synthesized materials were investigated by XRD, N2 adsorption, TEM, FT-IR pyridine, H2-TPR, and XPS. The size of ruthenium particles was found to be greatly dependent on the pretreatment gas (air or hydrogen) and the catalytic activity was enhanced by the small-size ruthenium metal nanoparticles, leading to changes in the reduction degree of ruthenium, which also increased the Brönsted and Lewis acidity. Metal to support charge transfer enhanced the reactant adsorption sites while oxygen vacancies on the interface enabled the dissociation of O2 molecules as revealed through DFT calculations. The outstanding catalytic activity of the 2Ru/TiO2 catalysts allowed to convert C3H8 into CO2 at reaction temperatures of about 100 °C. This high activity may be attributed to the metal/support interaction between Ru and TiO2, which promoted the reducibility of Ti4+/Ti3+ and Ru4+/Ru0 species, and to the fast migration of TiO2 lattice oxygen in the catalyst. Furthermore, the Ru/TiO2 catalyst exhibited high stability and reusability for 30 h under reaction conditions, using a GHSV of 45,000 h−1. The underlying alkane-metal interactions were explored theoretically in order to explain the C–H bond activation in propane by the catalyst.