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Effects of Ir-doping on the transition from oxidative coupling to partial oxidation of methane in La2O3-CeO2 nanofiber catalysts: spatial concentration and temperature profiles

机译:IR-掺杂对La2O3-CeO2纳米纤维催化剂中甲烷部分氧化氧化偶联的影响:空间浓度和温度曲线

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摘要

Spatially resolved temperature and species concentration profiles determined via microprobe sampling and online gas chromatography were used to examine the transition from oxidative coupling of methane (OCM) to catalytic partial oxidation (CPO) as a function of Ir-doping of a La2O3-CeO2 nanofiber fabric catalyst. Experiments were performed at atmospheric pressure at a furnace temperature of 750 degrees C, feed gas CH4/O-2 molar ratio of 5 and at a nominal space time of about 60 ms. Reaction products exhibited a dramatic shift from ethane and ethylene (OCM, C-2 selectivity of 54%), in the case of the un-doped catalyst, to exclusively synthesis gas (CPO, CO and H-2 selectivity 90+%), at 1% Ir doping. Species concentration profiles obtained in the latter case indicate the formation of H2O, H-2 and CO first, followed by the steam reforming of CH4 to produce the balance of the syngas concomitant with a sharp decrease in H2O levels. These findings suggest a CPO mechanism that is different from the literature, calling for the revision of detailed chemical kinetic mechanisms proposed before.
机译:通过微探针采样和在线气相色谱法测定的空间分辨温度和物种浓度分布用于检查从甲烷(OCM)的氧化偶联至催化部分氧化(CPO)的过渡,作为La2O3-CeO2纳米纤维织物的IR掺杂的函数催化剂。在750℃的炉温下在大气压下进行实验,进料气体CH4 / O-2摩尔比为5和在约60ms的标称空间时间。反应产物在未掺杂的催化剂的情况下,从乙烷和乙烯(OCM,C-2选择性为54%)的剧烈偏移,仅合成气体(CPO,CO和H-2选择性90 +%),以1%的红外掺杂。在后一种情况下获得的物种浓度谱表明,首先形成H 2 O,H-2和CO,然后进行CH4的蒸汽重整,以产生合成气的平衡,伴随着H2O水平的急剧下降。这些调查结果表明了一个与文献不同的CPO机制,呼吁修改之前提出的详细化学动力学机制。

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  • 来源
    《RSC Advances》 |2017年第43期|共7页
  • 作者单位

    Univ Calif Los Angeles Dept Chem &

    Biomol Engn Los Angeles CA 90095 USA;

    Univ Calif Los Angeles Dept Chem &

    Biomol Engn Los Angeles CA 90095 USA;

    Univ Calif Los Angeles Dept Chem &

    Biomol Engn Los Angeles CA 90095 USA;

    Kasetsart Univ Dept Chem Engn Fac Engn Bangkok 10900 Thailand;

    Univ Calif Los Angeles Dept Chem &

    Biomol Engn Los Angeles CA 90095 USA;

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  • 正文语种 eng
  • 中图分类 化学;
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