钴铝复合氧化物同时催化去除碳烟和氮氧化物

高等学校化学学报 ›› 2009, Vol. 30 ›› Issue (11): 2226.

钴铝复合氧化物同时催化去除碳烟和氮氧化物

王仲鹏^1,2, 张志翔², 上官文峰²

1. 济南大学化学化工学院, 济南 250022;
2. 上海交通大学燃烧与环境技术研究中心, 上海 200240

收稿日期:2009-01-08 出版日期:2009-11-10 发布日期:2009-11-10
通讯作者: 王仲鹏, 男, 博士, 讲师, 主要从事环境催化研究. E-mail: chm_wangzp@ujn.edu.cn
基金资助:
GM(通用汽车)-中国科学研究基金(批准号: 50222203)和济南大学博士基金(批准号: XBS0825)资助.

Cobalt-containing Hydrotalcites Derived Catalysts for Simultaneous Removal of NO_x and Soot

WANG Zhong-Peng^1,2*, ZHANG Zhi-Xiang², SHANGGUAN Wen-Feng²

1. School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China;
2. Research Center for Combustion and Environmental Technology, Shanghai Jiaotong University, Shanghai 200240, China

Received:2009-01-08 Online:2009-11-10 Published:2009-11-10
Contact: WANG Zhong-Peng. E-mail: chm_wangzp@ujn.edu.cn
Supported by:
GM(通用汽车)-中国科学研究基金(批准号: 50222203)和济南大学博士基金(批准号: XBS0825)资助.

摘要/Abstract

摘要：

以稳态共沉淀法合成的含Co类水滑石为前驱物, 制备了具有介孔结构的复合氧化物催化剂(CAO), 采用程序升温反应技术评价了催化剂同时去除碳烟和氮氧化物的性能, 并用ICP, BET, SEM和XPS等手段分析了材料结构和催化性能的关联. 结果表明, 催化剂呈现钴尖晶石相, 材料表面除了存在与金属键合的晶格氧外, 还有大量的吸附氧. Co/Al摩尔比和焙烧温度影响催化剂的活性, 当Co/Al摩尔比为4和焙烧温度为800 ℃时制备的4CAO-800是一种综合性能良好的催化剂, 具有较低的起燃温度(t_i=290 ℃), 生成N₂的选择性较高(S_N2/C=3.5%). 在同时去除碳烟和NO_x反应中, 碳烟的催化燃烧过程可能存在溢流机理和氧化还原机理协同作用.

关键词: 水滑石; 复合氧化物; 碳烟颗粒; 氮氧化物; 催化去除

Abstract:

Cobalt-containing mixed oxides(CAO) were prepared by thermal decomposition of hydrotalcite-like precursors with Co/Al molar ratio varying from 2 to 7. The catalytic activity of the CAO was investigated for the simultaneous catalytic removal of NO_x and diesel soot particulates by temperature-programmed reaction(TPR) technique in a fixed-bed flow reactor. The relationship between the catalyst structure and performance were clarified through ICP, BET, SEM and XPS measurements. The results show that all catalysts exhibit a nonstoichiometric spinel phase. Oxygen species present on the catalyst surface included lattice oxygen, the adsorbed oxygen and(or) the surface hydroxyl species, which acted for different mechanisms in soot oxidation. The catalytic activity was influenced by both Co/Al ratio and calcinations temperature. 4CAO-800 with the Co/Al molar ratio of 4 and calcinations temperature of 800 ℃ show the best activity with a low ignition tempe-rature(t_i=290 ℃) and high selectivity to N₂ formation(S_N2/C=3.5%). During the NO_x-soot reactions, a re-dox mechanism and a spillover mechanism may occur simultaneously for the catalytic soot oxidation.

Key words: Hydrotalcite; Mixed oxide; Soot particle; NO_x; Catalytic removal

TrendMD:

王仲鹏, 张志翔, 上官文峰. 钴铝复合氧化物同时催化去除碳烟和氮氧化物. 高等学校化学学报, 2009, 30(11): 2226.

WANG Zhong-Peng*, ZHANG Zhi-Xiang, SHANGGUAN Wen-Feng. Cobalt-containing Hydrotalcites Derived Catalysts for Simultaneous Removal of NO_x and Soot. Chem. J. Chinese Universities, 2009, 30(11): 2226.

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