Photothermal Synergistic Effect of Pt1/CuO-CeO2 Single-Atom Catalysts Significantly Improving Toluene Removal.

Photothermal synergistic catalytic oxidation of toluene over single-atom Pt catalysts was investigated. Compared with the conventional thermocatalytic oxidation in the dark, toluene conversion and CO2 yield over 0.39Pt1/CuO-CeO2 under simulated solar irradiation (λ = 320-2500 nm, optical power density = 200 mW cm-2) at 180 °C could be increased about 48%. An amount of CuO was added to CeO2 to disperse single-atom Pt with a maximal Pt loading of 0.83 wt %. The synergistic effect between photo- and thermocatalysis is very important for the development of new pollutant treatment technology with high efficiency and low energy consumption. Both light and heat played an important role in the present photothermal synergistic catalytic oxidation. 0.39Pt1/CuO-CeO2 showed good redox performance and excellent optical properties and utilized the full-spectrum solar energy. Light illumination induced the generation of reactive oxygen species (•OH and •O2-), which accelerated the transformation of intermediates, promoted the release of active sites on the catalyst surface, and improved the oxidation reaction.

Pd/silicalite-1: An highly active catalyst for the oxidative removal of toluene.

Catalytic combustion is thought as an efficient and economic pathway to remove volatile organic compounds, and its critical issue is the development of high-performance catalytic materials. In this work, we used the in situ synthesis method to prepare the silicalite-1 (S-1)-supported Pd nanoparticles (NPs). It is found that the as-prepared catalysts displayed a hexagonal prism morphology and a surface area of 390-440 m2/g. The sample (0.28Pd/S-1-H) derived after reduction at 500°C in 10 vol% H2 showed the best catalytic activity for toluene combustion (T50% = 180°C and T90% = 189°C at a space velocity of 40,000 mL/(g·hr), turnover frequency (TOFPd) at 160°C = 3.46 × 10-3 sec-1, and specific reaction rate at 160°C = 63.8 µmol/(gPd·sec)), with the apparent activation energy (41 kJ/mol) obtained over the best-performing 0.28Pd/S-1-H sample being much lower than those (51-70 kJ/mol) obtained over the other samples (0.28Pd/S-1-A derived from calcination at 500°C in air, 0.26Pd/S-1-im derived from the impregnation route, and 0.27Pd/ZSM-5-H prepared after reduction at 500°C in 10 vol% H2). Furthermore, the 0.28Pd/S-1-H sample possessed good thermal stability and its partial deactivation due to CO2 or H2O introduction was reversible, but SO2 addition resulted in an irreversible deactivation. The possible pathways of toluene oxidation over 0.28Pd/S-1-H was toluene â†’ p-methylbenzoquinone â†’ maleic anhydride, benzoic acid, benzaldehyde â†’ carbon dioxide and water. We conclude that the good dispersion of Pd NPs, high adsorption oxygen species concentration, large toluene adsorption capacity, strong acidity, and more Pd0 species were responsible for the good catalytic performance of 0.28Pd/S-1-H.