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The role of Pt-FexOy interfacial sites for CO oxidation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-12-08 , DOI: 10.1016/j.jcat.2017.11.021
Insoo Ro , Isaias B. Aragao , Joseph P. Chada , Yifei Liu , Keishla R. Rivera-Dones , Madelyn R. Ball , Daniela Zanchet , James A. Dumesic , George W. Huber

Supported Pt catalysts with different Fe/Pt atomic ratios were synthesized using controlled surface reactions to deposit (cyclohexadiene) iron tricarbonyl onto Pt/SiO2 to create Pt-FexOy interfacial sites. X-ray photoelectron spectroscopy measurements show that Pt and Fe species exist as metallic Pt and Fe oxides phases, respectively, after treatment in H2 at 573 K, whereas Fe becomes more oxidized under reaction conditions for CO oxidation at 313 K (CO:O2 = 1:1). The addition of Fe increases the turnover frequency of Pt1Fex/SiO2 at 313 K and atmospheric pressure by up to two orders of magnitude compared to Pt/SiO2. The reaction order with respect to the O2 partial pressure suggests that O2 adsorption on the surface is likely to be a rate controlling step for both Pt/SiO2 and Pt1Fe0.2/SiO2. The enhanced activity over Pt1Fex/SiO2 catalysts compared to Pt/SiO2 can be associated with a lower energy barrier for O2 adsorption and activation over Pt-FexOy interfacial sites.



中文翻译:

Pt-Fe x O y界面位对CO氧化的作用

使用受控的表面反应合成了具有不同Fe / Pt原子比的负载Pt催化剂,以将(环己二烯)三羰基铁沉积到Pt / SiO 2上以创建Pt-Fe x O y界面位。X射线光电子能谱测量表明,在573 K的H 2中处理后,Pt和Fe分别以金属Pt和Fe氧化物的形式存在,而Fe在313 K(CO:O 2  = 1:1)。的添加Fe的增加Pt组成的周转频率1的Fe X /二氧化硅2在313 K和大气压力高达两个数量级相比的Pt /二氧化硅2。关于O 2分压的反应顺序表明,对于Pt / SiO 2和Pt 1 Fe 0.2 / SiO 2,表面上的O 2吸附很可能是速率控制步骤。与Pt / SiO 2相比,Pt 1 Fe x / SiO 2催化剂的活性增强与在Pt-Fe x O y界面位上的O 2吸附和活化能较低。

更新日期:2017-12-08
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