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Highly selective production of syngas (>99%) in the partial oxidation of methane at 480 °C over Pd/CeO2 catalyst promoted by HCl
Applied Surface Science ( IF 6.7 ) Pub Date : 2021-05-07 , DOI: 10.1016/j.apsusc.2021.150043
Jeongeun Kim , Youngseok Ryou , Tae Hyeop Kim , Gyohyun Hwang , Jungup Bang , Jongwook Jung , Yongju Bang , Do Heui Kim

The partial oxidation of methane (POM) is an attractive catalytic route for producing syngas (CO/H2), although there are problems to overcome such as high reaction temperature (>650 °C) and the deactivation of the catalyst due to the coke formation. We addressed the problem by including HCl in the POM over a Pd/CeO2 catalyst. Pd/CeO2 produces CO, CO2, and coke with low CO selectivity in the absence of HCl, while it converts methane to chlorinated products at below 450 °C in the presence of HCl. At above 480 °C, however, highly selective CO (>99%) is produced over Pd/CeO2 via the POM. Moreover, it is found that coke is not formed during the reaction, leading to the stable partial oxidation activity and selectivity up to 40 h. Both surface and bulk characterization results strongly propose that HCl plays an essential role in transforming Pd/CeO2 into (PdClx + Pd0)/CeOCl (0 < x ≤ 2), which provides the ideal environment for the catalytic route of the POM.



中文翻译:

在HCl促进的Pd / CeO 2催化剂上,在480°C的甲烷部分氧化中,高选择性生产合成气(> 99%)

甲烷的部分氧化(POM)是生产合成气(CO / H 2)的有吸引力的催化途径,尽管存在诸如高反应温度(> 650°C)和由于焦炭导致催化剂失活等问题需要克服编队。我们通过在Pd / CeO 2催化剂上的POM中加入HCl解决了这一问题。在不存在HCl的情况下,Pd / CeO 2产生的CO,CO 2和焦炭的CO选择性低,而在HCl存在下,在低于450°C的温度下,Pd / CeO 2将甲烷转化为氯化产物。但是,在高于480°C的温度下,在Pd / CeO 2上会产生高选择性的CO(> 99%)通过POM。此外,发现在反应过程中不形成焦炭,导致​​稳定的部分氧化活性和选择性长达40小时。表面和本体表征结果都强烈建议HCl在将Pd / CeO 2转化为(PdCl x  + Pd 0)/ CeOCl(0 <x≤2)中起重要作用,这为POM的催化路线提供了理想的环境。 。

更新日期:2021-05-11
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