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Interaction Mechanism for Simultaneous Elimination of Nitrogen Oxides and Toluene over the Bifunctional CeO2–TiO2 Mixed Oxide Catalyst

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posted on 2022-03-07, 17:40 authored by Hao Liu, Jianjun Chen, Ya Wang, Rongqiang Yin, Wenhao Yang, Guimin Wang, Wenzhe Si, Yue Peng, Junhua Li
Simultaneous catalytic elimination of nitrogen oxides (NOx, x = 1 and 2) and volatile organic compounds (VOCs) is of great importance for environmental preservation in China. In this work, the interactions of simultaneous removal of NOx and methylbenzene (PhCH3) were investigated on a CeO2–TiO2 mixed oxide catalyst, which demonstrated excellent bifunctional removal efficiencies for the two pollutants. The results indicated that NOx positively promotes PhCH3 oxidation, while NH3 negatively inhibits through competitive adsorption with PhCH3. The underlying mechanism is that a pseudo PhCH3-SCR reaction happened in this process is parallel to NH3-SCR. Combined with in situ diffuse reflectance infrared Fourier transform spectroscopy and quasi in situ X-ray photoelectron spectroscopy, the interaction mechanism between NOx and PhCH3 is proposed. Specifically, NOx is adsorbed on the catalyst surface to produce nitrate species, which reacts with the carboxylate generated during PhCH3 oxidation to form organic nitrogen intermediates that create N2 and CO2 in the following reactions. In the reaction process, the superoxide (O2) generated by O2 activation on the catalyst surface is an important species for the propelling of oxidation reaction. This work could provide guidelines for the design of state-of-the-art catalysts for simultaneous catalytic removal of NOx and VOCs.

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