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Ceria-based catalysts for NOx removal in NSR processes: a fundamental study of the catalyst modifications explored by in situ techniques
Applied Surface Science ( IF 6.7 ) Pub Date : 2020-11-01 , DOI: 10.1016/j.apsusc.2020.147019
J.C. Martínez-Munuera , J. Giménez-Mañogil , L. Castoldi , L. Lietti , A. García-García

Abstract In this work, a fundamental and systematic study was conducted, leading to a better understanding of the phenomena occurring on the catalyst’s surface during the NOx reduction process in NSR systems. For this purpose, ceria-based catalysts, with Cu in substitution of noble metal, have been synthesized and deeply characterized by means of XRF, XPS, in situ (XRD, Raman spectroscopy and DRIFTS), temperature-programmed reduction under H2 (H2-TPR) and under NO reaction (NO isothermal reaction + NO-TPR). The whole results show the key role of copper to promote the reducibility and the creation of oxygen vacancies, allowing a high NO consumption and fast kinetics of N2O and N2 formation, until the oxygen vacancies consumption takes place. The study of the surface reactions taking place in the formation of adsorbed NOx species and the oxygen vacancies consumption with NO uptake is complex; however, a hydroxyl consumption route is found to be involved. The reduction of NO provided higher levels of N2 at higher temperatures; also, a very high efficiency of the previously created oxygen vacancies was found for this process.

中文翻译:

用于在 NSR 工艺中去除 NOx 的氧化铈基催化剂:通过原位技术探索的催化剂改性的基础研究

摘要 在这项工作中,进行了一项基础性和系统性的研究,从而更好地了解 NSR 系统中 NOx 还原过程中催化剂表面发生的现象。为此,已经合成了用 Cu 取代贵金属的氧化铈基催化剂,并通过 XRF、XPS、原位(XRD、拉曼光谱和漂移)、H2 下程序升温还原(H2- TPR)和在 NO 反应下(NO 等温反应 + NO-TPR)。整个结果表明,铜在促进还原性和氧空位产生方面的关键作用,允许高 NO 消耗和 N2O 和 N2 形成的快速动力学,直到发生氧空位消耗。对吸附的 NOx 物质形成过程中发生的表面反应和 NO 吸收的氧空位消耗的研究是复杂的;然而,发现涉及羟基消耗途径。NO 的还原在较高温度下提供了更高水平的 N2;此外,在该过程中发现先前产生的氧空位的效率非常高。
更新日期:2020-11-01
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