通过改良模板离子交换法将 MCM-41 和 MCM-48 与铜催化官能化,用于低温 NH3-SCR 过程:络合剂对铜分散的作用

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-10-09 DOI:10.1007/s11164-024-05414-2
Aleksandra Gomułka, Oliwia Iwaszko, Andrzej Kowalczyk, Zofia Piwowarska, Małgorzata Rutkowska, Lucjan Chmielarz
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引用次数: 0

摘要

通过模板离子交换(TIE)技术合成了 MCM-41 和 MCM-48 型介孔硅并对其进行了铜改性。随后用氨水、尿素或乙腈溶液处理样品,使沉积的铜物种高度分散。对铜改性硅的化学成分(ICP-OES)、多孔结构的有序性(XRD)、纹理参数(低温 N2 吸附)、引入铜物种的分散性和形态(UV-vis-DR、XRD、H2-TPR、NH3-TPD)进行了分析。铜修饰的介孔硅在氨选择性催化还原氮氧化物(NH3-SCR)中表现出良好的催化效率。与含有 CuO 团聚体的催化剂相比,含有分散铜物种(主要是单质铜阳离子)的样品具有更高的催化活性。另一方面,在氨被反应混合物中的氧气直接氧化的副反应过程中,CuO 聚合物表现出更高的催化活性。研究表明,用尿素对样品进行 TIE 后处理能最有效地改善沉积铜的分散性,与用氨溶液处理相比,对介孔二氧化硅有序多孔结构的破坏性更小。
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Catalytic functionalization of MCM-41 and MCM-48 with copper by modified template ion-exchange method for low-temperature NH3-SCR process: the role of complexing agents for copper dispersion

Mesoporous silicas of MCM-41 and MCM-48 types were synthesized and modified with copper by template ion-exchange (TIE) technique. A high dispersion of deposited copper species was managed by subsequent treatment of the samples with ammonia, urea, or acetonitrile solution. Copper-modified silicas were analysed in terms of their chemical composition (ICP-OES), ordering of porous structure (XRD), textural parameters (low-temperature N2 sorption), dispersion and form of introduced copper species (UV–vis-DR, XRD, H2-TPR, NH3-TPD). Mesoporous silicas modified with copper exhibited promising catalytic efficiency in selective catalytic reduction of NO with ammonia (NH3-SCR). The samples containing dispersed copper species (predominantly monomeric copper cations) presented enhanced catalytic activity compared to catalysts containing CuO aggregates. On the other hand, CuO aggregates showed greater catalytic activity in the side process of direct ammonia oxidation by oxygen present in the reaction mixture. It was demonstrated that TIE post-treatment of the samples with urea resulted in most effective improving dispersion of deposited copper and is less destructive for ordered porous structures of mesoporous silica comparing to treatment with ammonia solution.

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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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