In situ Raman study on the partial oxidation of methane to synthesis gas over Rh/Al2O3 and Ru/Al2O3 catalysts

In situ Raman study on the partial oxidation of methane to synthesis gas over Rh/Al2O3 and Ru/Al2O3 catalysts
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Rh/Al2O3 和 Ru/Al2O3 催化剂上甲烷部分氧化制合成气的原位拉曼研究

DOI:
10.1016/j.jcat.2008.03.009
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发表时间:
2008-06-10
影响因子:
7.3
通讯作者:
Wan, Hui-Lin
Wan, Hui-Lin
中科院分区:
化学1区
文献类型:
--
作者:
Liu, Ying;Huang, Fei-Yang;Wan, Hui-Lin

文献摘要

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利用原位显微探针拉曼和X射线衍射仪跟踪了甲烷部分氧化制合成气催化点火过程中Rh/Al_2O_3和Ru/Al_2O_3催化剂的氧化状态。结果表明,在POM反应开始前,催化剂处于完全氧化状态,在POM反应开始温度下,催化剂的氧化态发生突变。POM反应被点燃后,催化剂床层入口处催化剂中Rh_2O_3或RuO_2的含量低于拉曼光谱的检测水平。由于Ru-O的M-O键强度大于Rh-O,在POM条件下,Ru/Al_2O_3比Rh/Al_2O_3表现出更大的氧化倾向。这一因素会影响反应条件下两种催化剂上的氧覆盖率,进而影响合成气的生成途径。(C)2008 Elsevier Inc.保留所有权利。
In situ microprobe Raman and XRD techniques were used to follow the oxidation state of Rh/Al2O3 and Ru/Al2O3 catalysts during the catalytic ignition process of the partial oxidation of methane (POM) to synthesis gas. It was found that the catalyst was in the fully oxidized state before ignition of the POM reaction, and abruptly changed its oxidation state at the temperature at which the POM reaction started. After the POM reaction was ignited, the amount of Rh2O3 or RuO2 in the catalyst at the entrance of the catalyst bed was below the detection level of Raman spectroscopy. Due to the greater M-O bond strength of Ru-O compared with Rh-O, Ru/Al2O3 demonstrated a greater tendency to oxidize than Rh/Al2O3 under the POM conditions. This factor affects the oxygen coverage on the two catalysts under reaction conditions and consequently affects the pathways of synthesis gas formation. (c) 2008 Elsevier Inc. All rights reserved.