摘要
CH 3 Br catalytic oxidation as the probe reaction was investigated over Ru supported on TiO 2 with different crystalline phases. 1% Ru/anatase TiO 2 (a-TiO 2 ) exhibited superior stability at 240 °C after a 180 h time-on-stream run. And there was an induced activation for 1% Ru/a-TiO 2 during the initial 60 h reaction. Then the activity sustained stable. To elucidate the intrinsic mechanism, a series of characterizations were performed such as XRD, CO-Pulse, H 2 -TPR, XPS and NH 3 -TPD etc. Results showed that the Ru particle size increased and the Ru 0 content decreased as the reaction proceeded, which were not conductive to the reaction. It was assumed that the catalytic activity was strongly dependent on other factors. In combination with NH 3 -TPD and Py-FTIR measurements, it was confirmed that the enhanced activity and stability was strongly associated with the surface acidity, especially moderate strong Lewis acid (L acid). The increase of the acid amount and acidity strength was led by the generation and adsorption of HBr, Br 2 and RuO x Br y during the reaction, among which HBr and Br 2 was easier to desorb at 250 °C. While moderate strong L acid was sourced from the formation of RuO x Br y . The addition of transition metal (Ce, Co, Mn, Nb and Ni) further validated that the moderate strong L acid played a decisive role in the CH 3 Br catalytic oxidation.
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