Direct NO decomposition over conventional and mesoporous Cu-ZSM-5 and Cu-ZSM-11 catalysts: Improved performance with hierarchical zeolites

被引:117
作者
Kustova, M. Yu. [1 ]
Rasmussen, S. B. [1 ]
Kustov, A. L. [1 ]
Christensen, C. H. [1 ]
机构
[1] Tech Univ Denmark, Dept Chem, Ctr Sustainable & Green Chem, DK-2800 Lyngby, Denmark
关键词
NO decomposition; Cu-ZSM-5; Cu-ZSM-11; zeolite; mesopores; carbon; zeolite single crystals;
D O I
10.1016/j.apcatb.2006.04.014
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 [物理化学]; 081704 [应用化学];
摘要
Conventional Cu-ZSM-5 has for many years been recognized as a unique catalyst for direct NO decomposition. Zeolite-based catalysts have a crystallographically well-defined microporous structure. In such microporous catalysts, the creation and accessibility of the active sites is often influenced by the geometry of the pore system. To improve these catalysts, secondary mesoporous systems can benefitially be introduced into the structure of conventional zeolites. Here, this approach was used with Cu-containing ZSM-5 and ZSM-11 type mesoporous zeolite catalysts, which were used as catalysts for direct NO decomposition. It was discovered that introducing mesoporosity into the conventional materials leads to a significant improvement of the catalytic activity. Additionally, mesoporous Cu-ZSM-11 catalyst was found to be about twice as active as mesoporous Cu-ZSM-5. This difference is attributed to the fact that ZSM-11 has only straight microporous channels, while ZSNI-5 has both straight and sinusoidal channels. Apparently, there is a preferential formation of active sites and/or improved accessibility in the straight channels compared to the sinusoidal channels, which make the ZSM-11 material a better catalysts than ZSM-5. All samples were characterized by XRPD, SEM, TPD-NH3, in situ EPR and N-2 physisorption measurements. Thus, this confirms our previous observation that the special pore structure of Cu-ZSM-5 is not a decisive factor for the catalytic activity in NO decomposition. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:60 / 67
页数:8
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