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Highly dispersed CeO2on carbon nanotubes for selective catalytic reduction of NO with NH3

催化作用 X射线光电子能谱 选择性催化还原 材料科学 碳纳米管 解吸 大气温度范围 选择性 热脱附光谱法 吡啶 化学工程 无机化学 化学 纳米技术 吸附 物理化学 有机化学 工程类 物理 气象学
作者
Cheng Fang,Dengsong Zhang,Liyi Shi,Ruihua Gao,Hongrui Li,Liping Ye,Jianping Zhang
出处
期刊:Catalysis Science & Technology [Royal Society of Chemistry]
卷期号:3 (3): 803-811 被引量:160
标识
DOI:10.1039/c2cy20670f
摘要

Highly dispersed CeO2 on carbon nanotubes (CNTs) is successfully prepared by a pyridine-thermal route for selective catalytic reduction (SCR) of NO with NH3. This catalyst is mainly characterized by the techniques of X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction by hydrogen (H2-TPR), temperature-programmed desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS). The results of the XRD, TEM and TPR analysis show that the CeO2 particles on the CNTs are highly dispersed with a strong interaction between the particles and the CNTs. The NH3-TPD profiles indicate that this catalyst exhibits abundant strong acid sites. Furthermore, the O 1s XPS spectra show that the Oα/(Oα + Oβ) ratio of this catalyst is very high, which can result in more surface oxygen vacancies and therefore favor the NH3-SCR reaction. Compared with the catalysts prepared by impregnation or physical mixture methods, the catalyst prepared by the pyridine-thermal route presents the best NH3-SCR activity in the temperature range of 150–380 °C as well as favourable stability and good SO2 or H2O resistance. More than 90% of NO can be removed in the range of 250–370 °C with a desirable N2 selectivity. Moreover, the NO conversion can be kept at about 97% with the presence of SO2 or H2O at 300 °C. In addition, this catalyst shows a high catalytic activity with a NO conversion remaining constant at ca. 98% during a 16 h continuous run duration at 300 °C. Highly dispersed CeO2 on the CNTs as well as the strong interaction between the particles and the CNTs, the large amounts of strong acid sites and the high Oα/(Oα + Oβ) ratio could be ascribed to the excellent NH3-SCR performance of the catalyst prepared by the pyridine-thermal route.
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