不同钡铈比对NSR催化剂NO<sub><i>x</i></sub>存储性能的影响

王攀; 张博; 罗鹏; 孙川; 雷利利

不同钡铈比对NSR催化剂NO_x存储性能的影响

江苏大学汽车与交通工程学院, 江苏镇江 212013

基金项目:

国家自然科学基金 51676090

江苏省自然科学基金 BK20150513

江苏大学高级人才项目 14JDG152

详细信息

通讯作者:
王攀, Tel:13912809920, E-mail:wangpan@ujs.edu.cn

中图分类号: TK421⁺.5
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- 被引次数: 0
出版历程
- 收稿日期: 2017-04-27
- 修回日期: 2017-08-21
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-10-10

Effects of Ba/Ce ratio on NO_x storage performance of NSR catalyst

School of Automotive and Traffic Engineering, Jiangsu University, Zhenjiang 212013, China

Funds:

The project was supported by the National Natural Science Foundation of China 51676090

the Natural Science Foundation of Jiangsu BK20150513

the Advanced Talents' Foundation of Jiangsu University 14JDG152

摘要

摘要: 通过改进的溶胶凝胶法结合浸渍法制备了一系列Pt/x Ba-（30-x）Ce/γ-Al₂O₃（x=10、15、20，x为质量分数）型NSR催化剂，并利用XRD、BET、H₂-TPR和NO-TPD对其性能进行了表征。结果表明，Ba主要以BaCO₃形式存在，CeO₂晶粒粒径随着x值增大先减小后增大，且以无定型形式存在于催化剂中。随着Ce含量的增加，高温还原峰温度先降低后升高。NO-TPD结果表明，吸附于催化剂表面的NO_x在低温时具有较好的热稳定性；通过NO_x完全存储实验，探究了不同Ba/Ce比对催化剂NO_x存储性能的影响。结果表明，当x=15时，催化剂的NO_x存储量最大，NO_x穿透时间达7 min，吸附稳定时NO₂/NO_x比为28%，NO_x存储效率达47.1%，具有最佳的NO_x存储性能。
- 溶胶凝胶法 /
- NSR /
- NO_x存储性能 /
- Ba/Ce比 /
- 穿透时间
Abstract: In order to explore the effects of Ba/Ce ratio on the NO_x storage performance of the catalyst, a series of Pt/xBa-(30-x)Ce/γ-Al₂O₃ (x=10, 15, 20, x is a mass fraction) NSR catalysts were prepared by a modified sol-gel method combined with an impregnation method, and their properties were characterized by means of X-ray diffraction (XRD), specific surface area analysis (BET), temperature programmed reduction of H₂ (H₂-TPR) and temperature programmed desorption of NO (NO-TPD). The results indicate that Ba mainly exists in the form of BaCO₃, and CeO₂ is present in the amorphous form. With the increase of x value, CeO₂ grain size decreases firstly and then increases. With the increase of Ce content, the high temperature reduction peak has a similar tendency with that of CeO₂ grain size. The NO-TPD results show that the NO_x adsorbed on the surface of the catalyst has a better thermal stability with the temperature below 350℃. The effects of Ba/Ce ratio on the NO_x storage performance were investigated by a simulated gas test platform. The results show that the NO_x storage capacity of the Pt/15Ba-15Ce/γ-Al₂O₃ catalyst has a maximum value of 47.1%, and the NO_x breakthrough time is 7 min. When the storage process completes, the NO₂/NO_x ratio of Pt/15Ba-15Ce/γ-Al₂O₃ catalyst is 28%. The NO_x storage efficiency increases firstly and then decreases, and different Ba/Ce ratios have great influences on the storage path of the catalyst. The catalyst presents excellent NO_x storage performance when the Ba/Ce ratio is 1.0. The experimental results provide a reference for the optimal design and application of NSR catalyst in the field of diesel exhaust after-treatment system.
- sol-gel method /
- NO_x storage and reduction /
- NO_x storage performance /
- Ba/Ce ratio /
- breakthrough time

HTML全文

图 1 模拟实验台架装置示意图

Figure 1 Schematic of the simulated gas test platform

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图 2 Pt/xBa-(30-x)Ce/γ-Al₂O₃(x=10、15、20) 催化剂的XRD谱图

Figure 2 XRD patterns of Pt/xBa-(30-x)Ce/γ-Al₂O₃(x=10, 15, 20)

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图 3 NSR催化剂的H₂-TPR谱图

Figure 3 H₂-TPR profiles of NSR catalysts

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图 4 NSR催化剂的NO_x存储曲线

中文注解

Figure 4 NO_x storage patterns of NSR catalysts

(a): Pt/20Ba-10Ce/γ-Al₂O₃; (b): Pt/15Ba-15Ce/γ-Al₂O₃; (c): Pt/10Ba-20Ce/γ-Al₂O₃ ■: NO; ●: NO₂; ▲: NO_x

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图 5 不同Ba/Ce比的催化剂存储效率随时间的变化

Figure 5 NO_x storage efficiency of the catalysts with different Ba/Ce ratios as a function of storage time

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图 6 Pt/15Ba-15Ce/γ-Al₂O₃催化剂的NO-TPD谱图

Figure 6 NO-TPD profiles of Pt/15Ba-15Ce/γ-Al₂O₃ catalyst

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表 1 催化剂的比表面积以及孔容孔径

Table 1 BET and porous structure parameters of NSR catalysts

Catalyst	A_BET/(m²·g^-1)	Pore volume v/(cm³·g^-1)	Pore diameter d/ nm
Pt/20Ba-10Ce/γ-Al₂O₃	65.7	0.143	3.7
Pt/15Ba-15Ce/γ-Al₂O₃	91.8	0.147	3.6
Pt/10Ba-20Ce/γ-Al₂O₃	85.4	0.165	3.7
γ-Al₂O₃	211.4	0.232	3.8

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表 2 NSR催化剂的NO_x存储相关参数

Table 2 storage performance related parameters of NSR catalysts

Catalyst	NO_x storage efficiency /%	NO_x storage capacity/(μmol·g_cat^-1)	NO₂/NO_x	Breakthrough time t/min	Storage saturation time t/min
Pt/20Ba-10Ce/γ-Al₂O₃	40.1	358.04	20.96	5	40
Pt/15Ba-15Ce/γ-Al₂O₃	47.1	567.72	28	7	54
Pt/10Ba-20Ce/γ-Al₂O₃	41.68	297.71	20.16	3	32

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