低于300℃时两种氧化铈材料对稀燃阶段NO<sub><em>x</em></sub>存储性能的影响

引用本文: 朱金鑫, 沈美庆, 吕良方, 王军, 王建强. 低于300℃时两种氧化铈材料对稀燃阶段NO_x存储性能的影响[J]. 物理化学学报, 2014, 30(8): 1559-1566. doi: 10.3866/PKU.WHXB201405283 shu

Citation: 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 Physico-Chimica Sinica, 2014, 30(8): 1559-1566. doi: 10.3866/PKU.WHXB201405283 shu

低于300℃时两种氧化铈材料对稀燃阶段NO_x存储性能的影响

基金项目:
国家高技术研究发展计划项目（863）（2011AA03A405）资助

摘要:

研究了低于300 ℃时两种氧化铈对稀燃阶段NO_x存储性能的影响，催化剂由2%（w）Pt/Al₂O₃（PA）与CeO₂-X（X=S，I）机械混合制备. X射线衍射（XRD），BET表面积和扫描电子显微镜（SEM）用于表征材料的物理结构. X射线光电子能谱（XPS）和H₂程序升温还原（H₂-TPR）用于表面Ce³⁺和活性氧定量. 原位漫反射傅里叶变换红外光谱（in-situ DRIFTS）用于分析表面NO_x吸附物种. 相比于CeO₂-I，CeO₂-S 具有优良的物理化学性能，包括高比表面积、丰富的空隙结构、较高的抗老化能力及表面Ce³⁺浓度. 因而，Pt/Al₂O₃+CeO₂-S 表现出优异的NO_x存储能力. 此外，PA+CeO₂-X（X=S，I）上存在Pt 与CeO₂之间的相互作用，可提高表面氧物种的活性进而促进NO氧化及NO_x存储. PA+CeO₂-S上的这种相互作用要强于PA+CeO₂-I. 研究表明，表面Ce³⁺浓度和活性氧含量对NO_x存储起到重要作用. 然而经过水热处理后，Pt 与老化的氧化铈（ACS，ACI）之间的相互作用降低，并且两种氧化铈NO_x存储性能显著下降. 另外，与PA+ACS（ACI）相比，PA+PACS（PACI）样品NO_x存储能力得到改善，这归因于表面氧物种活性增加能促进硝酸盐的形成.

关键词:

English

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

1.
1. Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China
Received Date: 08 April 2014
Available Online: 18 July 2014
Fund Project:
国家高技术研究发展计划项目（863）（2011AA03A405）资助

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:

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沈阳化工大学材料科学与工程学院沈阳 110142

低于300℃时两种氧化铈材料对稀燃阶段NO_x存储性能的影响

English

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

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低于300℃时两种氧化铈材料对稀燃阶段NOx存储性能的影响

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