钯前驱体对汽车尾气处理Pd/Ce0.67Zr0.33O2催化剂催化性能的影响

doi:10.1016/S1872-2067(14)60264-3

催化学报 ›› 2015, Vol. 36 ›› Issue (4): 639-648.DOI: 10.1016/S1872-2067(14)60264-3

钯前驱体对汽车尾气处理Pd/Ce_0.67Zr_0.33O₂催化剂催化性能的影响

林嗣煜, 杨林颜, 阳雪, 周仁贤

浙江大学化学系催化研究所, 浙江杭州 310028

收稿日期:2014-10-29 修回日期:2014-12-12 出版日期:2015-03-23 发布日期:2015-03-23
通讯作者: Renxian Zhou
基金资助:
国家高技术研究发展计划(863计划, 2011AA03A406); 浙江省重点科技创新团队计划(2009R50020).

The effect of Pd precursor on Pd/Ce_0.67Zr_0.33O₂ catalysts for automotive emission control

Siyu Lin, Linyan Yang, Xue Yang, Renxian Zhou

Institute of Catalysis, Zhejiang University, Hangzhou 310028, Zhejiang, China

Received:2014-10-29 Revised:2014-12-12 Online:2015-03-23 Published:2015-03-23
Supported by:
This work was supported by the National High Technology Research and Development Program of China (863 Program, 2011AA03A406) and Zhejiang Leading Team of Science and Technology Innovation (2009R50020).

摘要/Abstract

摘要：

分别以Pd(NO₃)₂, Pd(NH₃)₄(NO₃)₂和H₂PdCl₄为钯前驱体制备了Pd/Ce_0.67Zr_0.33O₂ (CZ)催化剂. 以硝酸钯为钯前驱体制得的Pd/CZ(NO)催化剂具有较高的储氧量, 存在较多的小的钯簇, 其钯与载体间相互作用较强, 因此在三种新鲜催化剂中对HC和CO的消除表现出了最好的催化活性. 以硝酸四氨钯为钯前驱体制得的Pd/CZ(NH)催化剂具有较高的钯分散度, 存在较多的大的钯簇, 同时存在金属态和氧化态的钯, 从而对NO和NO₂的消除表现出了较好的催化活性. 以氯钯酸为钯前驱体制得的Pd/CZ(Cl)催化剂由于钯分散度较小, 钯与载体间作用较弱, 存在的CeOCl抑制了氧空穴的生成, 因此对各种反应物的催化活性都较低. 但Pd/CZ(Cl)催化剂表现出了较好的热稳定性, 这是由于老化处理消除了残余的氯物种并且促进了钯与载体间的作用.

关键词: 钯前驱体, 三效催化剂, 金属载体间相互作用, 起燃催化活性

Abstract:

A Pd/CZ(NO) catalyst prepared with Pd(NO₃)₂ as the metal precursor exhibited the best catalytic performance for HC and CO elimination because of a higher oxygen storage capacity, abundant small Pd_n clusters and a strong Pd-support interaction that facilitated electron transfer from PdO_x particles to the CZ support. A Pd/CZ(NH) catalyst prepared with Pd(NH₃)₄(NO₃)₂ as the metal precursor exhibited good performance for NO and NO₂ elimination due to a higher Pd dispersion, abundant bigger Pd_n clusters and oxidized/metallic Pd coexistence. A Pd/CZ(Cl) catalyst prepared with H₂PdCl₄ as the metal precursor exhibited low catalytic activity due to a low Pd dispersion, weak Pd-support interaction, and the trace amount of CeOCl which inhibited oxygen vacancy creation. However, it showed good thermal stability, and benefited when an aging treatment removed the residual chlorine species and also promoted the interaction between PdO_x and the support.

Key words: Palladium precursor, Three-way catalyst, Noble metal-support interaction, Light-off catalytic performance

林嗣煜, 杨林颜, 阳雪, 周仁贤. 钯前驱体对汽车尾气处理Pd/Ce_0.67Zr_0.33O₂催化剂催化性能的影响[J]. 催化学报, 2015, 36(4): 639-648.

Siyu Lin, Linyan Yang, Xue Yang, Renxian Zhou. The effect of Pd precursor on Pd/Ce_0.67Zr_0.33O₂ catalysts for automotive emission control[J]. Chinese Journal of Catalysis, 2015, 36(4): 639-648.

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钯前驱体对汽车尾气处理Pd/Ce_0.67Zr_0.33O₂催化剂催化性能的影响

The effect of Pd precursor on Pd/Ce_0.67Zr_0.33O₂ catalysts for automotive emission control

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