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CoCeOx-PVP Catalyst for Effective CO-SCR in the Presence of O2
Yuansong Zhou1, Fengyu Gao1, Lei Yi1
1Beijing Key Laboratory of Resource-Oriented Treatment of Industrial Pollutants, School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China.
Abstract:
In an O2-containing environment, achieving efficient selective catalytic reduction of nitrogen oxides (NOx) by carbon monoxide (CO) using non-noble metal catalysts remains a formidable challenge. To balance the catalytic oxidation of CO and the catalytic reduction of NOx, we need to develop a catalyst with strong reductibility and weak oxidizability for the CO selective catalytic reduction of NOx (CO-SCR) reaction in the presence of O2. In this study, we synthesized the CoCeOx-PVP catalyst via a coprecipitation method and employed various characterization techniques, including BET, SEM, XRD, Raman, XPS, H2-TPR, and O2-TPD. The analysis results indicate that the addition of polyvinylpyrrolidone (PVP) alters the surface structure of the catalyst, increases the particle size, and enhances the concentration of surface oxygen vacancies. These structural effects facilitate electron circulation and accelerate the migration of oxygen species, thereby improving the catalytic reduction performance of the catalyst and increasing the conversion rate of NOx. At 250 °C and with 5 vol% O2, the conversion rates of NOx and CO can attain 98% and 96%, respectively, accompanied by a remarkable N2 selectivity of 99%. Following a sustained reaction period of 6 h, the conversion efficiencies of both NOx and CO remain above 95%. However, during extended testing periods, as the oxygen vacancies are progressively occupied by O2, the oxygen vacancies generated through the reduction of NO with CO fall short of sustaining the CO-SCR reaction over the long haul. Subsequently, the oxidation reactions of NO and CO come to dominate, resulting in a decline in the NOx conversion rate. Notably, the CO conversion rate still maintains 100% at this point. Based on the results of in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) experiments, we proposed a reaction mechanism for the CO-SCR process over the CoCeOx-PVP catalyst under O2-containing conditions. This study provides an effective strategy for the application of non-noble metal catalysts in the field of CO-SCR. Although maintaining long-term activity of the catalyst remains a challenge in the presence of O2, the catalyst in this study exhibits a slower deactivation rate compared to traditional non-noble metal catalysts.
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