浸渍钾的铜铝催化剂在利用 CO 还原 NO 和 N2O 过程中的性能

IF 5.2 2区 化学 Q1 CHEMISTRY, APPLIED
Suelen Martins Stutz Gomes, Samara da Silva Montani, Luz Amparo Palacio, Fatima Maria Zanon Zotin
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引用次数: 0

摘要

三元汽车催化剂(TWC)以贵金属为基础,有两个显著的局限性:成本高,在低温下容易形成一氧化二氮(N2O),导致温室效应和臭氧层破坏。因此,研究这些成分的可能替代品至关重要。在这项工作中,研究了用钾浸渍铜和铝氢铝酸盐类材料制备的催化剂。催化剂中水滑石相和氧化铜相的形成由 X 射线衍射 (XRD) 证明。温度编程还原(TPR)结果表明,碱金属会对催化剂的还原性产生积极影响,降低其还原温度。温度编程解吸(TPD)分析显示了电子促进作用,证实钾的存在促进了表面分子氮的解吸,降低了 N2O 的解吸。催化测试表明,催化剂的行为因所进行的预处理而有所不同,这表明钾与氧化铜或还原铜之间的相互作用产生了不同的催化位点。经 XPS 鉴定,含钾催化剂中氧空位的形成和铜金属表面积的增加有助于解释为什么这些催化剂具有更好的性能。此外,根据催化测试,添加了钾(最大程度地减少了 N2O 的形成)的催化剂具有更高的选择性,特别是在钾/铜(摩尔/摩尔)比率为 0.025 时和经过还原预处理后。在温度接近 100 ℃ 时,这种催化剂在一氧化碳还原过程中的一氧化二氮转化率也达到了 100%,证明了它在减少一氧化二氮方面的卓越性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Performance of copper-aluminum catalysts impregnated with potassium in NO and N2O reduction by CO
Three-way automotive catalysts (TWC) are based on noble metals and have two significant limitations: high cost and tendency to form, at low temperatures, nitrous oxide (N2O), which contributes to the greenhouse effect and ozone layer depletion. Thus, it is crucial to study possible substitutes for these components. In this work, catalysts prepared from copper and aluminum hydrotalcite-like materials impregnated with potassium were studied. The formation of the hydrotalcite phase and CuO phase in the catalyst was evidenced by X-ray diffraction (XRD). Temperature-programmed reduction (TPR) results showed that the alkali metal positively influences the reducibility of the catalyst, decreasing its reduction temperature. Temperature-programmed desorption (TPD) analysis revealed electronic promotion, confirming that the presence of potassium facilitates the desorption of molecular nitrogen from the surface and decreases that of N2O. Catalytic tests showed differences in the behavior of the catalysts depending on the pretreatment performed, suggesting that the interaction between potassium and oxidized or reduced copper gives rise to different catalytic sites. The formation of oxygen vacancies in potassium-containing catalysts, identified by XPS, and the increase in the copper metal surface area contributed to explaining the better performance of these catalysts. Also, based on the catalytic tests, more selective catalysts with the addition of potassium (minimizing N2O formation) were obtained, especially at a ratio of 0.025 K/Cu (mol/mol) and after a reducing pretreatment. This catalyst also showed 100 % N2O conversion in the reduction by CO at temperatures close to 100 °C, confirming its excellent performance in nitrous oxide abatement.
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来源期刊
Catalysis Today
Catalysis Today 化学-工程:化工
CiteScore
11.50
自引率
3.80%
发文量
573
审稿时长
2.9 months
期刊介绍: Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.
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