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

• Published in: Environmental science and pollution research international Vol. 30; no. 43; pp. 98076 - 98090
• Main Authors: Camposeco, Roberto, Miguel, Omar, Torres, Ana E., Armas, Daniela E., Zanella, Rodolfo
• Format: Journal Article
• Language: English
• Published: Berlin/Heidelberg Springer Berlin Heidelberg 01-09-2023; Springer Nature B.V
• Subjects: Acidity; Adsorption; Alkanes; Aquatic Pollution; Atmospheric Protection/Air Quality Control/Air Pollution; Carbon dioxide; Catalysis; Catalysts; Catalytic activity; Catalytic converters; Catalytic oxidation; Charge transfer; Earth and Environmental Science; Ecotoxicology; Environment; Environmental Chemistry; Environmental Health; Hydrogen bonds; Metals; Nanoparticles; Oxidation; Oxygen; Physicochemical properties; Propane; Research Article; Ruthenium; Titanium dioxide; Urea; Waste Water Technology; Water Management; Water Pollution Control; H; oxidation; C–H bond dissociation; Ruthenium; C; TiO
• ISSN: 1614-7499; 0944-1344; 1614-7499
• DOI: 10.1007/s11356-023-29153-w

Ruthenium is a robust catalyst for a variety of applications in environmental heterogeneous catalysis. The catalytic performance of Ru/TiO
2
materials, synthesized by using the deposition precipitation with urea method, was assessed in the catalytic oxidation of C
3
H
8
, 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, N
2
adsorption, TEM, FT-IR pyridine, H
2
-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 O
2
molecules as revealed through DFT calculations. The outstanding catalytic activity of the 2Ru/TiO
2
catalysts allowed to convert C
3
H
8
into CO
2
at reaction temperatures of about 100 °C. This high activity may be attributed to the metal/support interaction between Ru and TiO
2
, which promoted the reducibility of Ti
4+
/Ti
3+
and Ru
4+
/Ru
0
species, and to the fast migration of TiO
2
lattice oxygen in the catalyst. Furthermore, the Ru/TiO
2
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.