Pt-Ni/CNTs-γ-Al2O3用于富氢气体中CO的优先氧化

摘要

通过胶溶法制备碳纳米管(CNTs)-γ-Al₂O₃复合材料,并以其为载体,采用共浸渍法制备一系列Pt-Ni双金属催化剂用于富氢气体中CO优先氧化。采用N₂物理吸附脱附、X射线衍射(XRD)、H₂-程序升温还原(H₂-TPR)、透射电子显微镜(TEM)、扫描透射电子显微镜(STEM)和扫描电子显微镜(SEM)技术对催化剂进行了表征。在低温条件下,Pt-Ni/CNTs-γ-Al₂O₃催化剂在CO优先氧化反应中表现出高的活性和选择性,并具有宽的净化CO温度窗口。复合材料中的CNTs被氧化铝包裹,低温条件下还原所得Pt-Ni合金纳米颗粒均匀分布在Al₂O₃表面。该催化剂优良的催化性能归因于Pt-Ni合金的形成和CNTs的添加避免或减缓了热点的形成。热点的存在导致氧气用于H₂氧化的选择性提高,并且会促使逆水汽变换反应的发生,两者均对CO的消除有害。

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	安继民
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	刘源

关键词：碳纳米管氧化铝铂氢优先氧化

Abstract：

The carbon nanotubes (CNTs)-γ-alumina composite was prepared by colloidal processing. A series of CNTs-γ-alumina composite supported platinum-nickel catalysts were prepared by co-impregnation method and were applied to the preferential oxidation(PROX) of CO in H₂-rich gases. The catalysts were characterized by N₂ adsorption-desorption, X-Ray diffractions(XRD), H₂-temperature programmed reduction(H₂-TPR), transmission electron microscopy(TEM), scanning transmission electron microscopy (STEM) and scanning electron microscopy(SEM). The catalyst of Pt-Ni/CNTs-γ-Al₂O₃ exhibited very high activity and selectivity with broad temperature window for CO removal via PROX at low temperature. The Pt-Ni alloy species which can be reduced at low temperature are highly dispersed on the support. CNTs in the composite were wrapped and the nanoparticles of Pt-Ni were on the surface of Al₂O₃. The very good catalytic performance of this catalyst is attributed to the formation of Pt-Ni alloy as well as the addition of CNTs, which can avoid or mitigate the formation of hotspots. The hotspots can increase the selectivity of oxygen to H₂ oxidation and can generate reverse water gas shift reaction, both of which are harmful for eliminating CO.

Keywords： carbon nanotubes； alumina； platinum； hydrogen； preferential oxidation

Received 2014-03-19;

Fund:

国家自然科学基金(21376170,21263011);国家教育部博士点专项基金(20100032110019)。

Corresponding Authors: 刘源,E-mail:yuanliu@tju.edu.cn。 Email: yuanliu@tju.edu.cn

About author: 安继民(1987-),男,硕士研究生,从事应用催化方面的研究。

引用本文:

安继民, 钮挺, 刘源.Pt-Ni/CNTs-γ-Al₂O₃用于富氢气体中CO的优先氧化[J]. 化学工业与工程, 2016,33(2): 7-16

An Jimin, Niu Ting, Liu Yuan.Carbon Nanotubes-γ-Alumina Composite Supported Pt-Ni Catalysts for Preferential Oxidation of CO in H₂-Rich Gases[J]. Chemcial Industry and Engineering, 2016,33(2): 7-16

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