低于300℃时两种氧化铈材料对稀燃阶段NOx存储性能的影响

doi:10.3866/PKU.WHXB201405283

Abstract

Abstract:

The present work investigated the effects of two types of CeO₂ materials on the lean NO_x trap (LNT) performance over NO_x storage reduction (NSR) catalysts below 300 ℃. These materials were obtained by mechanical mixing of 2% (w) Pt/Al₂O₃ (PA) with CeO₂-X (X=S, I). X-ray diffraction (XRD), BET surface area measurements, and scanning electron microscopy (SEM) were used to characterize the physical structures of the catalysts, while X-ray photoelectron spectroscopy (XPS) and H₂ temperature-programmed reduction (H₂-TPR) were employed to identify and quantify the surface Ce³⁺ concentrations and the amounts of surface-active oxygen. In-situ diffuse reflectance infrared Fourier transform spectroscopy (In-situ DRIFTS) was applied to analyze the surface adsorbed NO_x species. Compared with CeO₂-I, CeO₂-S presented superior physico-chemical properties, including higher surface area, richer porous texture, stronger aging-resistance, and higher surface Ce³⁺ concentration. As a result, the PA+CeO₂-S sample also exhibited outstanding NO_x trapping capacity. Furthermore, interaction between Pt and CeO₂ was observed in the PA+CeO₂-X mixtures, which facilitates NO oxidation and the NO_x trapping process owing to the accompanying increase in the activity of surface active oxygen on the CeO₂. This interaction was stronger in the case of the PA+CeO₂-S sample as compared with the PA+CeO₂-I. The Ce³⁺ content and presence of active oxygen species on the CeO₂ surface both play critical roles in the NO_x trapping process and hydrothermal treatment of the CeO₂ significantly decreased the NO_x trapping capacity of both PA+CeO₂ samples. It was also determined that the interaction between Pt and aged CeO₂ is weakened and that the NO_x trapping capacity of aged CeO₂ is enhanced after loading a small amount of Pt, which is attributed to the promotion of nitrate formation by increased surface oxygen activity.

Key words: NO_x storage and reduction catalyst, Ceria material, Pt metal, Lean NO_x trap capacity, Physical-chemical property, Surface-active oxygen, Interaction

ZHU Jin-Xin, SHEN Mei-Qing, Lü Liang-Fang, WANG Jun, WANG Jian-Qiang. Effects of Two Different CeO₂ Materials on Lean NO_x Trap Performance below 300 ℃[J]. Acta Phys. -Chim. Sin. 2014, 30(8), 1559-1566. doi: 10.3866/PKU.WHXB201405283

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Effects of Two Different CeO₂ Materials on Lean NO_x Trap Performance below 300 ℃

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Effects of Two Different CeO₂ Materials on Lean NO_x Trap Performance below 300 ℃