Developing high-performance Pt-based catalysts with low Pt loading is crucial but challenging for CO oxidation at temperatures below 100 °C. Herein, we report a Pt-based catalyst with only a 0.15 wt% Pt loading, which consists of Pt–Ti intermetallic single-atom alloy (ISAA) and Pt nanoparticles (NP) co-supported on a defective TiO2 support, achieving a record high turnover frequency of 11.59 s–1 at 80 °C and complete conversion of CO at 120 °C. This is because the coexistence of Pt–Ti ISAA and Pt NP significantly alleviates the competitive adsorption of CO and O2, enhancing the activation of O2. Furthermore, Pt single atom sites are stabilized by Pt–Ti ISAA, resulting in distortion of the TiO2 lattice within Pt–Ti ISAA. This distortion activates the neighboring surface lattice oxygen, allowing for the simultaneous occurrence of the Mars-van Krevelen and Langmuir–Hinshelwood reaction paths at low temperatures.
In this work, ruthenium-based bimetallic catalysts of the formula Ru–5M/TiO2 (M = Mn, Co, Ce, Cu, Fe) were prepared and evaluated in benzene oxidation, and Ru–5Co/TiO2 exhibited the lowest complete oxidation temperature (220 °C), demonstrating Co3O4 as the best dopant. The influence of the Ru and Co contents on the catalytic activity was also studied, and 1 wt% Ru and 5 wt% Co3O4 were confirmed. Water vapor showed an inhibition effect on benzene oxidation at 210 °C, whereas the catalytic efficiency was barely influenced at a higher temperature (230 °C). STEM analyses revealed that Ru–Co bimetallic species showed similar distributions on the catalytic surface. Based on the correlation of the catalytic results with various characterization techniques, the synergistic effect between Ru and Co was well demonstrated, and a four-step transformation in the oxidation process was concluded. Besides, systematic in situ FTIR studies for benzene oxidation over Ru/TiO2, Co/TiO2, and Ru–5Co/TiO2 were conducted and compared, and many organic intermediates were observed in the in situ FTIR spectra. Accordingly, the reaction mechanism for benzene oxidation over the Ru–Co bimetallic catalyst was proposed.
24 March 2021 in Environmental Science and Pollution Research