富氢气氛下CO选择性氧化催化剂Pt/γ-Al2O3中添加钴的作用

化学学报 ›› 2004, Vol. 62 ›› Issue (21): 2143-2149. 上一篇下一篇

研究论文

富氢气氛下CO选择性氧化催化剂Pt/γ-Al₂O₃中添加钴的作用

严菁¹, 马建新², 周伟²

1. 华东理工大学工业催化研究所, 上海, 200237;
2. 同济大学新能源汽车工程中心, 上海, 200092

投稿日期:2004-02-09 修回日期:2004-04-28 发布日期:2014-02-17
通讯作者: jxma@fcv-sh.com
作者简介:马建新,Email:jxma@fcv-sh.com;Fax:(021)69589461

Effect of Cobalt in Modifying Pt/γ-Al₂O₃ Catalyst for Preferential Oxidation of CO in Hydrogen-rich Stream

YAN Jing¹, MA Jian-Xin², ZHOU Wei²

1. Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237;
2. Clean Energy Automotive Engineering Center, Tongji University, Shanghai 200092

Received:2004-02-09 Revised:2004-04-28 Published:2014-02-17

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摘要/Abstract

研究了Pt/γ-Al₂O₃催化剂上添加Co对降低Pt负载量的效应,同时通过XRD,CO-TPD,H₂-TPR和FTIR等手段对Co助催的Pt/γ-Al₂O₃催化剂进行了表征,藉此探讨了Co的改性作用.实验结果表明,在Pt/γ-Al₂O₃催化剂中添加Co可显著降低Pt的用量和改善低温活性.在Pt负载量为w_Pt=0.01,Co添加量为w_Co=0.015～0.03时,在ψ_O₂/ψ_CO=1.0和120℃的较低温度下,CO转化率和O₂选择性分别高达99%和47%以上.在Pt/γ-Al₂O₃催化剂中添加的Co以不完全还原的CoO_x形态存在,不仅可以提供活泼氧与CO反应生成CO₂,而且影响Pt的电子性能,使之较难还原.Co的引入还削弱了CO在Pt上的吸附,使CO线式吸附物种消失,同时使碳酸氢盐和甲酸盐吸附物种增加.随温度升高,Co/Pt/γ-Al₂O₃催化剂上碳酸氢盐物种消失并转化成CO₂.

关键词: 选择性氧化, 一氧化碳, 富氢气氛, 钴, Pt/γ-Al₂O₃, 燃料电池

Carbon monoxide is a poison to the Pt anode in proton exchange membrane fuel cell (PEMFC). Preferential oxidation (PROX) over Pt/γ-Al₂O₃ catalyst is an effective method to reduce CO in hydrogen rich gas streams to a tolerant level. In this paper, the effect of adding Co to Pt/γ-Al₂O₃ catalyst on lowering Pt-loading and improving catalytic properties was investigated. Experimental results showed that the addition of Co to Pt/γ-Al₂O₃ could not only improve the activity at low-temperature but also reduce significantly the Pt-loading in the catalysts. Over the catalysts with Pt-loading of w_Pt=0.01 and Co loading of w_Co=0.015～0.03 and in the conditions of temperature at 120℃ and φ_O₂ /φ_CO=1.0, the conversion of CO could reach over 99% and the selectivity of O₂ was 47%. The results of characterization by XRD, CO-TPD, H₂-TPR and FTIR revealed that in the promoted catalyst there existed incompletely reduced cobalt oxides, which not only provided active oxygen to CO to the formation of CO₂ but also affected the electronic property of Pt, leading to a more difficult reduction of Pt. Furthermore, the addition of Co weakened the adsorption of CO on Pt, inhibited the linear adsorption of CO on Pt, and increased the surface adsorption of bicarbonate and formate species. Bicarbonate species diminished quickly and turned into CO₂ over Co/Pt/γ-Al₂O₃ with increasing temperature.

Key words: preferential oxidation, carbon monoxide, hydrogen-rich stream, cobalt, Pt/γ-Al₂O₃,fuel cell

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严菁, 马建新, 周伟. 富氢气氛下CO选择性氧化催化剂Pt/γ-Al₂O₃中添加钴的作用[J]. 化学学报, 2004, 62(21): 2143-2149.

YAN Jing, MA Jian-Xin, ZHOU Wei. Effect of Cobalt in Modifying Pt/γ-Al₂O₃ Catalyst for Preferential Oxidation of CO in Hydrogen-rich Stream[J]. Acta Chimica Sinica, 2004, 62(21): 2143-2149.

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富氢气氛下CO选择性氧化催化剂Pt/γ-Al₂O₃中添加钴的作用

Effect of Cobalt in Modifying Pt/γ-Al₂O₃ Catalyst for Preferential Oxidation of CO in Hydrogen-rich Stream

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