MnOx对Pt/CeZrO2催化剂在水汽和CO2环境下CO氧化的影响

doi:10.11949/j.issn.0438-1157.20170942

化工学报 ›› 2018, Vol. 69 ›› Issue (4): 1484-1492.DOI: 10.11949/j.issn.0438-1157.20170942

• 催化、动力学与反应器 • 上一篇下一篇

MnO_x对Pt/CeZrO₂催化剂在水汽和CO₂环境下CO氧化的影响

朱丽¹, 邓芸¹, 宋宇鹏², 王月娟¹, 鲁继青¹, 罗孟飞¹

1. 浙江师范大学物理化学研究所, 浙江金华 321004;
2. 金华职业技术学院化工与制药学院, 浙江金华 321017

收稿日期:2017-07-24 修回日期:2017-09-27 出版日期:2018-04-05 发布日期:2018-04-05
通讯作者: 罗孟飞
基金资助:
浙江省公益技术应用研究项目（2016C31SA700016）。

Effect of MnO_x on Pt/CeZrO₂ catalyzed CO oxidation under water vapor and CO₂ conditions

ZHU Li¹, DENG Yun¹, SONG Yupeng², WANG Yuejuan¹, LU Jiqing¹, LUO Mengfei¹

1. Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang, China;
2. School of Chemical and Pharmaceutical Engineering, Jinhua Polytechnic, Jinhua 321017, Zhejiang, China

Received:2017-07-24 Revised:2017-09-27 Online:2018-04-05 Published:2018-04-05
Supported by:
supported by the Public Welfare Technology Application Research Project of Zhejiang Province (2016C31SA700016).

摘要/Abstract

摘要：

以CeZrO₂固溶体为载体，发现MnO_x的添加能促进Pt/CeZrO₂催化剂的CO氧化性能，并研究了MnO_x含量对催化剂CO氧化活性及抗H₂O和CO₂性能的影响。结果表明，随着MnO_x含量增加，催化剂活性呈现先升高后降低的趋势，在MnO_x含量为0.5%（质量分数）时活性最佳。MnO_x的添加降低了Pt颗粒尺寸并影响催化剂还原性能从而促进反应活性。水汽和CO₂对Pt/CeZrO₂催化剂的CO氧化活性有抑制作用，而MnO_x的加入能显著提高催化剂的抗水汽和CO₂的能力。反应动力学结果表明，在Pt/CeZrO₂催化剂上，反应气中引入H₂O和CO₂后，CO的反应级数有明显升高，说明H₂O和CO₂在催化剂表面与CO竞争吸附，导致CO反应活性下降；而在Pt/MnO_x/CeZrO₂催化剂上，CO的反应级数略有升高，说明MnO_x的添加能有效抑制H₂O和CO₂与CO的竞争吸附，从而改善了催化剂的抗H₂O和CO₂性能。

关键词: Pt催化剂, CO氧化, MnO_x, 动力学

Abstract:

Adding MnO_x to CeZrO₂ solid solution carrier could effectively enhance Pt/CeZrO₂ catalyst activity for CO oxidation. The effect of the amount of MnO_x on catalytic activity and resistance of H₂O and CO₂ was studied. The results showed that the activity of Pt/MnO_x/CeZrO₂ catalyst was first increased and then decreased as MnO_x content was increased with a maximum activity at 0.5% (mass) MnO_x content. The addition of MnO_x improved catalyst activity by reducing Pt particle size and changing catalyst reducibility. The presence of H₂O vapor and CO₂ in feed gas suppressed activity of Pt/CeZrO₂ catalyst, which was effectively alleviated by MnO_x in the catalyst. Kinetic study revealed that CO reaction order was considerably increased with presence of H₂O and CO₂for the Pt/CeZrO₂ catalyst. Such a decline of catalyst activity might be due to competitive adsorption of H₂O and CO₂ over CO on catalyst surface. In contrast, the CO reaction order was slightly increased with presence of H₂O and CO₂ for Pt/0.5MnO_x/CeZrO₂ catalyst, implying that addition of MnO_x could suppress competitive adsorption of H₂O and CO₂ over CO on catalyst surface and hence improve resistance to H₂O and CO₂.

Key words: Pt catalysts, CO oxidation, MnO_x, kinetics

中图分类号:

O643.3

朱丽, 邓芸, 宋宇鹏, 王月娟, 鲁继青, 罗孟飞. MnO_x对Pt/CeZrO₂催化剂在水汽和CO₂环境下CO氧化的影响[J]. 化工学报, 2018, 69(4): 1484-1492.

ZHU Li, DENG Yun, SONG Yupeng, WANG Yuejuan, LU Jiqing, LUO Mengfei. Effect of MnO_x on Pt/CeZrO₂ catalyzed CO oxidation under water vapor and CO₂ conditions[J]. CIESC Journal, 2018, 69(4): 1484-1492.

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MnO_x对Pt/CeZrO₂催化剂在水汽和CO₂环境下CO氧化的影响

Effect of MnO_x on Pt/CeZrO₂ catalyzed CO oxidation under water vapor and CO₂ conditions

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