CeO2的添加对柴油车氧化催化剂Pt/SiO2-Al2O3的NO氧化性能提高的影响

引用本文: 黄于芬, 张海龙, 杨铮铮, 赵明, 黄木兰, 梁艳丽, 王健礼, 陈耀强. CeO₂的添加对柴油车氧化催化剂Pt/SiO₂-Al₂O₃的NO氧化性能提高的影响[J]. 物理化学学报, 2017, 33(6): 1242-1252. doi: 10.3866/PKU.WHXB201703292 shu

Citation: HUANG Yu-Fen, ZHANG Hai-Long, YANG Zheng-Zheng, ZHAO Ming, HUANG Mu-Lan, LIANG Yan-Li, WANG Jian-Li, CHEN Yao-Qiang. Effects of CeO₂ Addition on Improved NO Oxidation Activities of Pt/SiO₂-Al₂O₃ Diesel Oxidation Catalysts[J]. Acta Physico-Chimica Sinica, 2017, 33(6): 1242-1252. doi: 10.3866/PKU.WHXB201703292 shu

CeO₂的添加对柴油车氧化催化剂Pt/SiO₂-Al₂O₃的NO氧化性能提高的影响

黄于芬 ^1, ,
张海龙 ^2, ,
杨铮铮 ^3, ,
赵明 ^1, ,
黄木兰 ^1, ,
梁艳丽 ^1, ,
王健礼 ^1, ,
陈耀强 ^1,

1.
四川大学化学学院, 绿色化学与技术教育部重点实验室, 成都 610064;
2.
四川大学化学工程学院, 成都 610064;
3.
西华师范大学环境科学与工程学院, 四川南充 637009
基金项目:
国家自然科学基金（21173153）和国家高技术研究发展计划项目（863）（2015AA034603）资助

摘要: 采用分步浸渍法制备不同CeO₂含量改性SiO₂-Al₂O₃载体的Pt/SiO₂-Al₂O₃柴油车氧化催化剂Pt/SiO₂-Al₂O₃-wCeO₂（质量分数w为0%，5%，10%，15%，30%）。利用固定床反应器，在模拟柴油车行驶条件下测定催化反应活性。活性结果表明，无论CO和C₃H₆存在与否，适量CeO₂的添加均明显提高了Pt/SiO₂-Al₂O₃柴油车氧化催化剂的NO氧化性能。其中，Pt/SiO₂-Al₂O₃-15% CeO₂表现出了最优氧化性能，其能在较宽温度范围内维持61%的NO₂产率。CO-化学吸附结果表明，适量CeO₂的添加有利于提高Pt的分散度，即提高催化剂表面可利用Pt原子比例。透射电镜（TEM）结果证实了CeO₂改性后高分散的Pt颗粒的存在，X射线衍射（XRD）结果也说明CeO₂改性后的载体更利于抑制Pt晶粒的增长。氢气程序升温还原（H₂-TPR）和TEM结果均说明CeO₂的添加增强了贵金属-载体间的相互作用，从而更利于PtOx与CeO₂还原。总之，本文表明CeO₂改性柴油车催化剂（DOC）可以提高催化剂的分散性和还原性，从而提高NO催化氧化性能，其对工业应用中柴油车尾气净化后处理复合系统（DOC+DPF+SCR）的净化效率的提高有重要意义。

关键词:

English

Effects of CeO₂ Addition on Improved NO Oxidation Activities of Pt/SiO₂-Al₂O₃ Diesel Oxidation Catalysts

1.
Key Laboratory of Green Chemistry & Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China;
2.
College of Chemical Engineering, Sichuan University, Chengdu 610064, P. R. China;
3.
College of Environmental Science and Engineering, China West Normal University, Nanchong 637009, Sichuan Province, P. R. China
Received Date: 12 December 2016
Revised Date: 13 March 2017
Available Online: 29 March 2017
Fund Project:
The project was supported by the National Natural Science Foundation of China (21173153) and National Hi-Tech Research and Development Program of China (863) (2015AA034603).

Abstract: The catalytic activities for NO oxidation achieved by different amounts of CeO₂-modified Pt/SiO₂-Al₂O₃ catalysts Pt/SiO₂-Al₂O₃-wCeO₂ (the mass fraction w being 0%, 5%, 10%, 15%, 30%), prepared using step-wise impregnation, were investigated in the presence and absence of CO and C₃H₆. The results showed that the NO oxidation activity could be efficiently improved by modification of CeO₂, wherein the 15%-CeO₂-modified catalyst exhibited the maximum NO conversion of 61% even in the presence of CO and C₃H₆, which were proved to inhibit NO₂ formation in this study. A series of characterization methods were performed over the as-prepared samples to correlate their surface and structural characteristics with their enhanced NO oxidation activities. CO-chemisorption illustrated that appropriate CeO₂-loading was effective for enhancing Pt dispersion, thus enhancing Pt surface-to-volume ratio, confirmed by transmission electron microscope (TEM) images. X-Ray Diffraction (XRD) further suggested that ceria addition could suppress the growth of the Pt crystal, resulting in higher surface Pt atomic ratio. Further, H₂ temperature-programmed reduction (H₂-TPR), together with TEM results, implied that the presence of ceria could enhance the interaction between metal and supports, thus facilitating reducibility of both active platinum and ceria. Hence, this study displays that ceria could act as a dispersion promoter and a reducibility booster, both of which are beneficial to NO oxidation activity. The improved NO oxidation activity is significant for the efficient purification of diesel integrated catalytic system.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

CeO₂的添加对柴油车氧化催化剂Pt/SiO₂-Al₂O₃的NO氧化性能提高的影响

English

Effects of CeO₂ Addition on Improved NO Oxidation Activities of Pt/SiO₂-Al₂O₃ Diesel Oxidation Catalysts

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