Praseodymium effects on great improving low-temperature hydrothermal stability of Cu/SAPO-34 NH3-SCR catalysts

IF 5.2 1区 化学 Q1 CHEMISTRY, APPLIED Journal of Rare Earths Pub Date : 2024-03-01 DOI:10.1016/j.jre.2024.02.009
Xiaojie Yu, Xinyu Li, Chen Wang, Jianqiang Wang, Meiqing Shen, M.D. Tarikul Islam, Gurong Shen
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Abstract

Based on the previous findings that the presence of hydroxyl groups on the outer surface is crucial for maintaining skeletal stability, we propose a strategy modified Cu/SAPO-34 using Pr ions in this study. Therefore, we conducted several measurements to investigate the effect of Pr ions on the low-temperature hydrothermal stability of Cu/SAPO-34. We find that Pr exists only on the surface of Cu/SAPO-34 as ions and oxides, with Pr ions playing a protective role in occupying surface acidic sites. The addition of small amounts of Pr leads to the re-dispersion of Cu, resulting in improved low-temperature selective catalytic reduction (SCR) activity in the as-synthesized samples. Furthermore, it enhances the resistance to decomposition of the Si–(OH)–Al framework during low-temperature hydrothermal aging, thereby preserving the framework structure and allowing detached active Cu species to return to exchangeable positions, ultimately restoring SCR activity. However, as the Pr content increases, the enhanced acidity causes some structural damage, gradually weakening the protective effect. Our work demonstrates that Pr modification is a simple and effective solution to the issue of poor low-temperature hydrothermal stability in Cu/SAPO-34, providing a promising way for the application of light rare earth elements.
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镨对大幅提高 Cu/SAPO-34 NH3-SCR 催化剂低温水热稳定性的影响
根据之前的研究结果,即外表面羟基的存在对于维持骨架稳定性至关重要,我们在本研究中提出了一种使用 Pr 离子改性 Cu/SAPO-34 的策略。因此,我们进行了多项测量,研究 Pr 离子对 Cu/SAPO-34 低温水热稳定性的影响。我们发现,Pr 只以离子和氧化物的形式存在于 Cu/SAPO-34 的表面,Pr 离子在占据表面酸性位点方面起着保护作用。添加少量 Pr 会导致铜重新分散,从而提高合成样品的低温选择性催化还原 (SCR) 活性。此外,在低温水热老化过程中,它还能增强 Si-(OH)-Al 框架的抗分解能力,从而保留框架结构,并使分离的活性 Cu 物种返回到可交换位置,最终恢复 SCR 活性。然而,随着 Pr 含量的增加,酸性的增强会造成一些结构破坏,从而逐渐削弱保护作用。我们的工作表明,Pr 改性是解决 Cu/SAPO-34 低温水热稳定性差问题的一种简单而有效的方法,为轻稀土元素的应用提供了一种前景广阔的途径。
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来源期刊
Journal of Rare Earths
Journal of Rare Earths 化学-应用化学
CiteScore
8.70
自引率
14.30%
发文量
374
审稿时长
1.7 months
期刊介绍: The Journal of Rare Earths reports studies on the 17 rare earth elements. It is a unique English-language learned journal that publishes works on various aspects of basic theory and applied science in the field of rare earths (RE). The journal accepts original high-quality original research papers and review articles with inventive content, and complete experimental data. It represents high academic standards and new progress in the RE field. Due to the advantage of abundant RE resources of China, the research on RE develops very actively, and papers on the latest progress in this field emerge every year. It is not only an important resource in which technicians publish and obtain their latest research results on RE, but also an important way of reflecting the updated progress in RE research field. The Journal of Rare Earths covers all research and application of RE rare earths including spectroscopy, luminescence and phosphors, rare earth catalysis, magnetism and magnetic materials, advanced rare earth materials, RE chemistry & hydrometallurgy, RE metallography & pyrometallurgy, RE new materials, RE solid state physics & solid state chemistry, rare earth applications, RE analysis & test, RE geology & ore dressing, etc.
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