Influence of the synthesis route on the catalytic oxidation of 1,2-dichloroethane over CeO2/H-ZSM5 catalysts

Influence of the synthesis route on the catalytic oxidation of 1,2-dichloroethane over CeO2/H-ZSM5 catalysts
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DOI:
10.1016/j.apcata.2013.02.026
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发表时间:
2013-04-10
影响因子:
5.5
通讯作者:
Gutierrez-Ortiz, J. I.
Gutierrez-Ortiz, J. I.
中科院分区:
化学2区
文献类型:
--
作者:
de Rivas, B.;Sampedro, C.;Gutierrez-Ortiz, J. I.

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对标称 CeO2 负载量为 10 wt.% 的负载型 CeO2/HZSM-5 催化剂的性能进行了评估,以评估废物流中最常见的氯化污染物之一(即 1,2-二氯乙烷)的氧化情况。考察了不同介质(水和乙醇)浸渍、沉淀和离子交换等制备方法的影响。通过原子发射光谱、X射线衍射、BET测量、透射电子显微镜、X射线光电子能谱、NH3程序升温解吸、低温吸附CO然后红外光谱、程序升温氢还原、能量色散X射线光谱和动态热重分析与质谱联用,分析了合成过程引起的结构、形态和物理化学变化。相对于普通 H-ZSM5,所得二氧化铈负载样品的催化行为的增强可以基于氧迁移率和酸位点的协同效应来解释。特别是,基于乙醇浸渍的方法产生了具有大量氧空位的高度分散的二氧化铈催化剂。因此,该催化剂需要低于 200 摄氏度的温度才能实现 50% 的转化率。 (C) 2013 Elsevier B.V. 保留所有权利。
The performance of supported CeO2/HZSM-5 catalysts with a nominal CeO2 loading of 10 wt.% was evaluated for the oxidation of one of the most common chlorinated pollutants found in waste streams, namely 1,2-dichloroethane. The influence of the preparation method, such as impregnation in different media (water and ethanol), precipitation and ion exchange, was examined. Structural, morphological and physico-chemical changes caused as a function of the synthesis procedure were analysed by atomic emission spectroscopy, X-ray diffraction, BET measurements, transmission electronic microscopy, X-ray photoelectron spectroscopy, NH3-temperature-programmed desorption, adsorption of CO at low temperature followed by infrared spectroscopy, temperature-programmed reduction with hydrogen, energy dispersive X-ray spectroscopy and dynamic thermogravimetry coupled to mass spectrometry. The enhancement of the catalytic behaviour of the resulting ceria loaded samples with respect to plain H-ZSM5 could be explained on the basis of the synergetic effects of oxygen mobility and acid sites. In particular, the procedure based on impregnation with ethanol led to a highly dispersed ceria catalyst with a larger amount of oxygen vacancies. As a result, this catalyst required a temperature lower than 200 degrees C for attaining 50% conversion. (C) 2013 Elsevier B.V. All rights reserved.