Pt/Ce0.6Zr0.4O2催化剂催化氧化碳烟过程中活性氧对NO-NO2循环及表面含氧物种的分解作用

doi:10.1016/S1872-2067(14)60004-8

催化学报 ›› 2014, Vol. 35 ›› Issue (3): 407-415.DOI: 10.1016/S1872-2067(14)60004-8

Pt/Ce_0.6Zr_0.4O₂催化剂催化氧化碳烟过程中活性氧对NO-NO₂循环及表面含氧物种的分解作用

刘爽, 吴晓东, 林雨, 李敏, 翁端

清华大学材料学院先进材料教育部重点实验室, 北京100084

收稿日期:2013-11-09 修回日期:2013-12-13 出版日期:2014-02-26 发布日期:2014-02-26
通讯作者: 吴晓东
基金资助:
国家自然科学基金（51072096）；国家重点基础研究发展计划（973计划，2010CB732304）；国家高技术研究发展计划（863计划，2013AA065302）.

Active oxygen-assisted NO-NO₂ recycling and decomposition of surface oxygenated species on diesel soot with Pt/Ce_0.6Zr_0.4O₂ catalyst

Shuang Liu, Xiaodong Wu, Yu Lin, Min Li, Duan Weng

Key Laboratory of Advanced Materials of MOE, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Received:2013-11-09 Revised:2013-12-13 Online:2014-02-26 Published:2014-02-26
Supported by:
This work was supported by the National Natural Science Foundation of China (51072096), the National Basic Research Program of China (973 Program, 2010CB732304), and the National High Technology Research and Development Program of China (863 Program, 2013AA065302).

摘要/Abstract

摘要：

通过在Ce_0.6Zr_0.4O₂载体上浸渍Pt（NO₃）₂制得Pt/Ce_0.6Zr_0.4O₂催化剂，该催化剂在松散接触条件下，于NO+O₂或O₂气氛中均表现出比Pt/Al₂O₃更好的碳烟氧化性能. 进一步研究表明，Pt/Ce_0.6Zr_0.4O₂催化剂中的Pt 与Ce_0.6Zr_0.4O₂存在相互作用，使得催化剂在一定温度范围内对活性氧的利用率大为提高，从而促进了气氛中NO↔NO₂的循环，乃至碳烟与NO₂的反应和碳烟表面含氧中间物种的生成；更重要的是，这部分活性氧本身可加速含氧中间物种的分解. 因此，在NO + O₂的气氛中，Pt/Ce_0.6Zr_0.4O₂催化剂的碳烟起燃温度比Pt/Al₂O₃降低了34 ℃.

关键词: 铂催化剂, 铈锆复合氧化物, 碳烟氧化, 一氧化氮-二氧化氮循环, 表面含氧物种

Abstract:

A Pt/Ce_0.6Zr_0.4O₂ catalyst was synthesized by impregnating a Ce_0.6Zr_0.4O₂ support with Pt(NO₃)₂ solution. This material exhibits higher catalytic activity than Pt/Al₂O₃ for soot oxidation under loose contact conditions in both NO + O₂ and O₂ atmospheres. The results show that the pronounced activity of this catalyst is attributed to a synergistic effect arising from the combination of Pt and Ce_0.6Zr_0.4O₂ solid solution, leading to a remarkable increase in the availability of active oxygen at temperatures as low as 450 ℃. The NO↔NO₂ recycling efficiency is improved over Pt/Ce_0.6Zr_0.4O₂ catalyst, enhancing the ability of the NO₂-soot reaction to generate surface oxygenated complexes (SOCs) on the soot. More importantly, the catalytic oxidation of these SOCs can be accelerated with the participation of active oxygen from the CeO₂-ZrO₂ solid solution. As a result, during soot oxidation under NO + O₂, the light-off temperature of the Pt/Ce_0.6Zr_0.4O₂ catalyst is lowered by 34 ℃ than that of Pt/Al₂O₃ catalyst.

Key words: Platiumn-based catalyst, Ceria-zirconia mixed oxide, Soot oxidation, Nitrogen monoxide-nitrogen dioxide recycling, Surface oxygenated species

刘爽, 吴晓东, 林雨, 李敏, 翁端. Pt/Ce_0.6Zr_0.4O₂催化剂催化氧化碳烟过程中活性氧对NO-NO₂循环及表面含氧物种的分解作用[J]. 催化学报, 2014, 35(3): 407-415.

Shuang Liu, Xiaodong Wu, Yu Lin, Min Li, Duan Weng. Active oxygen-assisted NO-NO₂ recycling and decomposition of surface oxygenated species on diesel soot with Pt/Ce_0.6Zr_0.4O₂ catalyst[J]. Chinese Journal of Catalysis, 2014, 35(3): 407-415.

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Pt/Ce_0.6Zr_0.4O₂催化剂催化氧化碳烟过程中活性氧对NO-NO₂循环及表面含氧物种的分解作用

Active oxygen-assisted NO-NO₂ recycling and decomposition of surface oxygenated species on diesel soot with Pt/Ce_0.6Zr_0.4O₂ catalyst

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