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Zr 改性的 Cu/ZSM-5 催化剂上用于 NH₃ 选择性催化还原 NO 时对钙中毒的抗性增强

Enhanced resistance to calcium poisoning on Zr-modified Cu/ZSM-5 catalysts for the selective catalytic reduction of NO with NH.

作者信息

Xue Hongyan, Meng Tao, Liu Fangfang, Guo Xiaoming, Wang Shengdong, Mao Dongsen

机构信息

Research Institute of Applied Catalysis, School of Chemical and Environmental Engineering, Shanghai Institute of Technology Shanghai 201418 PR China

Shanghai Institute for Design & Research in Environmental Engineering Co., Ltd. Shanghai 200232 PR China.

出版信息

RSC Adv. 2019 Nov 25;9(66):38477-38485. doi: 10.1039/c9ra07722g.

Abstract

Ca/ZrCu/ZSM-5 catalysts containing different Zr contents were prepared by incipient wetness impregnation. The catalysts were tested for the selective catalytic reduction (SCR) of NO with ammonia and characterized by N-BET, NO titration, XRD, NH-TPD, H-TPR, and XPS techniques. In the temperature range of 100-170 °C, after calcium impregnation, NO conversion over the Cu/ZSM-5 catalyst decreased by 11.3-24.3%, while that over Zr/Cu/ZSM-5 only decreased by 3.8-12.2%. The improvement of the calcium poisoning resistance of the ZrCu/ZSM-5 catalyst is mainly attributed to an increase in the dispersion and the surface concentration of Cu. Moreover, the addition of zirconium promotes the reduction of CuO by decreasing the interaction between CuO and CaO, which also contributes to the improvement of resistance to CaO poisoning. The apparent activation energy and turnover frequency for the SCR reaction over the Ca/Zr Cu/ZSM-5 catalysts were calculated and discussed.

摘要

采用初湿浸渍法制备了不同锆含量的Ca/ZrCu/ZSM-5催化剂。对这些催化剂进行了氨选择性催化还原(SCR)NO的测试,并采用N-BET、NO滴定、XRD、NH-TPD、H-TPR和XPS技术对其进行了表征。在100 - 170°C温度范围内,浸渍钙后,Cu/ZSM-5催化剂上的NO转化率降低了11.3 - 24.3%,而Zr/Cu/ZSM-5催化剂上的NO转化率仅降低了3.8 - 12.2%。ZrCu/ZSM-5催化剂抗钙中毒性能的提高主要归因于Cu的分散度和表面浓度的增加。此外,锆的加入通过降低CuO与CaO之间的相互作用促进了CuO的还原,这也有助于提高抗CaO中毒性能。计算并讨论了Ca/ZrCu/ZSM-5催化剂上SCR反应的表观活化能和转化频率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52a4/9075838/d3fbe11b8d00/c9ra07722g-f1.jpg

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