Oscillatory Behavior of Pd-Au Catalysts in Toluene Total Oxidation

Abstract

In this work, the activity of bimetallic Pd-Au doped hierarchically structured titania catalysts has been investigated in the total oxidation of toluene. In earlier works, doping titania with group Vb metal oxides ensured an increased catalytic performance in the elimination of VOC molecules. A synergy between gold and palladium loaded at the surface of titania supports provided better performances in VOC oxidation reactions. Therefore, the main focus in this work was to investigate the durability of the prepared catalysts under long time-on-stream periods. Vanadium-doped catalysts showed a stable activity throughout the whole 110 h test, whereas, surprisingly, niobium-doped catalysts presented a cycle-like activity while nevertheless maintaining a high performance in toluene elimination. Operando Diffuse Reflectance Infrared Fourrier Transform spectroscopy (DRIFT) experiments revealed that variations in the presence of OH radicals and the presence of carbonaceous compounds adsorbed at the surface of spent catalysts varies with the occurrence of oscillations. X-ray Photoelectron Spectroscopy (XPS) results show that interactions between the material and the active phase provided extra amounts of mobile oxygen species and participated in easing the reduction of palladium. An enhanced redox reaction scheme is thus obtained and allows the occurrence of the cyclic-like performance of the catalyst.