Promotional effects of phosphotungstic acid on CePO4 catalyst for the selective catalytic reduction of NO with NH3

催化作用 磷钨酸 化学 氮氧化物 氧化还原 选择性催化还原 无机化学 路易斯酸 双功能 吸附 核化学 有机化学 燃烧
作者
Lantian Zhang,Ran Zhao,Hongxia Li,Jinxiao Bao,Qingchun Wang
出处
期刊:Molecular Catalysis [Elsevier]
卷期号:551: 113666-113666
标识
DOI:10.1016/j.mcat.2023.113666
摘要

CePO4 was prepared using the co-precipitation method. Recognizing the bifunctional nature of hetero-polyacid (salt), with both acidic and redox properties, it was modified by using phosphotungstic acid (HPW), and the HPW/CePO4 catalysts were synthesized using the impregnation technique. Various advanced techniques were employed to investigate aspects such as catalytic activity, microstructure, surface properties, and reaction mechanisms. These methods included NH3-SCR, XRD, XPS, SEM, BET, NH3-TPD, H2-TPR, and In-situ DRIFTs. Experimental findings indicated that the HPW-modified CePO4 catalysts exhibited enhanced SCR activity. Among them, the reaction activity window for NOx conversion of the W: Ce 0.05 catalyst was found to be 300∼400 °C, which represented the best activity temperature window. Following the incorporation of HPW, the HPW/CePO4 catalysts demonstrated an increased presence of Brønsted acidic sites, which concurrently led to a significant reduction in SO2 adsorption. The W: Ce 0.05 catalyst possessed the highest ratios of Oα/(Oα+Oβ+Oγ) and Ce4+/(Ce3++Ce4+). These ratios effectively regulated the sequestration and release of reactive oxygen species, thereby enhancing the activation of NH3. Consequently, this promoted the catalyst's low-temperature NH3-SCR reactivity. Lastly, the reaction process was examined using in-situ DRIFTs. The study revealed the generation of -NH2 intermediates at the Lewis acid sites of the W: Ce 0.05 catalyst. These intermediates subsequently underwent reactions with gaseous NO via the Eley-Rideal mechanism. This approach not only amplified the low-temperature catalytic efficacy of the catalysts but also bolstered their resilience to SO2, thereby fostering the long-term stability of the NH3-SCR reaction.
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