Y对柴油车碳烟氧化催化剂MnOx-CeO2热稳定性的影响

doi:10.1016/S1872-2067(15)60867-1

催化学报 ›› 2015, Vol. 36 ›› Issue (8): 1333-1341.DOI: 10.1016/S1872-2067(15)60867-1

Y对柴油车碳烟氧化催化剂MnO_x-CeO₂热稳定性的影响

张海龙^a, 王健礼^a, 曹毅^a, 王益静^b, 龚茂初^a, 陈耀强^a,c

a 四川大学化学学院, 绿色化学与技术教育部重点实验室, 四川成都610064;
b 宁波远翔节能环保技术有限公司, 浙江宁波315800;
c 四川省环境催化材料工程技术中心, 四川成都610064

收稿日期:2015-02-26 修回日期:2015-04-14 出版日期:2015-07-29 发布日期:2015-07-30
通讯作者: 陈耀强
基金资助:
国家高技术研究发展计划(863计划, 2013AA065304); 绿色催化四川省高校重点实验室开放课题(2013LF3004).

Effect of Y on improving the thermal stability of MnO_x-CeO₂ catalysts for diesel soot oxidation

Hailong Zhang^a, Jianli Wang^a, Yi Cao^a, Yijing Wang^b, Maochu Gong^a, Yaoqiang Chen^a,c

a Key Laboratory of Green Chemistry and Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China;
b Ningbo Yuanxiang Energy Saving and Environmental Protection Technology Company, Ningbo 315800, Zhejiang, China;
c Sichuan Provincial Environmental Catalytic Material Engineering Technology Center, Chengdu 610064, Sichuan, China

Received:2015-02-26 Revised:2015-04-14 Online:2015-07-29 Published:2015-07-30
Supported by:
This work was supported by the National High Technology Research and Development Program of China (863 Program, 2013AA065304) and the Open Object for Green Catalysis and Key Laboratory of Sichuan Provincial University (2013LF3004).

摘要/Abstract

摘要：

采用共沉淀法制备了不同Y含量的MnO_x-CeO₂-Y₂O₃催化剂, 并用于NO_x存在条件下的碳烟氧化反应. 通过在干空气气流中800 ℃焙烧12 h评价了这些催化剂的热稳定性. 采用X射线衍射、N₂吸附-脱附、拉曼光谱、H₂程序升温还原、储氧量测试、NO程序升温氧化、X射线光电子能谱和碳烟程序升温氧化等手段对催化剂进行了表征. 实验发现, Y的添加导致催化剂比表面积、还原性能和储氧能力下降, 从而影响了NO和碳烟的氧化活性. 然而, 热老化之后, Y可增大催化剂的热稳定性, 其中以6%-10% Y的添加效果最好, 它们的最大碳烟氧化速率温度仅增加了34-35 ℃. MnO_x-CeO₂催化剂的催化活性和热失活与其表面的Mn⁴⁺和氧物种密切相关.

关键词: MnO_x-CeO₂-Y₂O₃, 碳烟氧化活性, 热稳定性, 氧化还原性质, 氧储存能力

Abstract:

A series of MnO_x-CeO₂-Y₂O₃ catalysts with different Y loadings (0, 1, 3, 6, and 10 wt%) were prepared by a co-precipitation method and investigated for NO_x-assisted soot oxidation. The thermal stabilities of these catalysts were evaluated by treating them at 800 ℃ for 12 h under dry air flow. The catalysts were characterized by X-ray diffraction, N₂ adsorption-desorption, Raman spectroscopy, H₂ temperature-programmed reduction, oxygen storage capacity, NO temperature- programmed oxidation, X-ray photoelectron spectroscopy, and soot temperature-programmed oxidation. The addition of Y led to decreased BET surface areas and poor low-temperature reduction abilities and oxygen storage capacities, which affected NO and soot oxidation activities. However, after aging, the doping of Y had effectively enhanced the stability of the catalytic activities for NO and soot oxidations, where the addition of 6%-10% Y achieved the optimum result because the maximal soot oxidation rate temperature was increased by only 34-35 ℃. Additionally, the catalytic activity and deactivation of MnO_x-CeO₂-containing catalysts were closely related to the presence of Mn⁴⁺ and oxygen species on the surface.

Key words: MnO_x-CeO₂-Y₂O₃, Soot oxidation activity, Thermal stability, Redox property, Oxygen storage capacity

张海龙, 王健礼, 曹毅, 王益静, 龚茂初, 陈耀强. Y对柴油车碳烟氧化催化剂MnO_x-CeO₂热稳定性的影响[J]. 催化学报, 2015, 36(8): 1333-1341.

Hailong Zhang, Jianli Wang, Yi Cao, Yijing Wang, Maochu Gong, Yaoqiang Chen . Effect of Y on improving the thermal stability of MnO_x-CeO₂ catalysts for diesel soot oxidation[J]. Chinese Journal of Catalysis, 2015, 36(8): 1333-1341.

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Y对柴油车碳烟氧化催化剂MnO_x-CeO₂热稳定性的影响

Effect of Y on improving the thermal stability of MnO_x-CeO₂ catalysts for diesel soot oxidation

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