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Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-01-03 , DOI: 10.1016/j.jcat.2017.12.011
Aiyong Wang , Yilin Wang , Eric D. Walter , Ravi K. Kukkadapu , Yanglong Guo , Guanzhong Lu , Robert S. Weber , Yong Wang , Charles H.F. Peden , Feng Gao

Fe/zeolites are important N2O abatement catalysts, efficient in direct N2O decomposition and (selective) catalytic N2O reduction. In this study, Fe/Beta and Fe/SSZ-13 materials were synthesized via solution ion-exchange and used to catalyze these two reactions. The nature of the Fe species was probed with UV–vis, Mössbauer and EPR spectroscopies and H2-TPR. These characterizations collectively indicate that primarily isolated and dinuclear Fe sites are present in Fe/SSZ-13, whereas Fe/Beta contains higher concentrations of oligomeric FexOy species. H2-TPR results suggest that Fe-O interactions are weaker in Fe/SSZ-13, as evidenced by the lower reduction temperatures by H2 and higher extents of autoreduction during high-temperature pretreatments in inert gas. Kinetic measurements show that Fe/SSZ-13 has higher normalized reaction rates in catalytic N2O decomposition, thus demonstrating a positive correlation between reaction rate and Fe-O binding, consistent with O2 desorption being rate-limiting for this reaction. However, Fe/Beta was found to display higher reaction rates in catalyzing N2O reduction by NH3. This latter result indicates that larger active ensembles (i.e., oligomers) are responsible for this reaction, consistent with the fact that both N2O and NH3 need to be activated in this case.



中文翻译:

Fe / Beta和Fe / SSZ-13催化剂催化N 2 O分解和NH 3还原

铁/沸石是重要Ñ 2 ö减排催化剂,直接氮高效2 ö分解和(选择性的)催化正2 O简化。在这项研究中,通过溶液离子交换合成了Fe / Beta和Fe / SSZ-13材料,并用于催化这两个反应。用UV-vis,Mössbauer和EPR光谱仪以及H 2 -TPR探测了Fe物种的性质。这些特征共同表明,Fe / SSZ-13中主要存在分离的双核Fe位点,而Fe / Beta包含较高浓度的低聚Fe x O y物种。高2-TPR结果表明,Fe / SSZ-13中的Fe-O相互作用较弱,这可由较低的H 2还原温度和在惰性气体中进行高温预处理期间较高的自动还原程度来证明。动力学测量表明,Fe / SSZ-13在催化N 2 O分解中具有更高的归一化反应速率,因此证明了反应速率与Fe-O结合之间呈正相关,这与O 2解吸是该反应的速率限制相一致。然而,发现Fe / Beta在催化NH 3还原N 2 O时显示出更高的反应速率。后一个结果表明较大的活性集合体(即低聚物)负责该反应,这与两个N在这种情况下,需要激活2 O和NH 3

更新日期:2018-01-03
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