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Spectroscopic characterization of Mn-Co-Ce mixed oxides,active catalysts for COPROX reaction

机译:Mn-Co-Ce混合氧化物,COPROX反应活性催化剂的光谱表征

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摘要

Mn-Co-Ce mixed oxides are active and selective catalysts for the CO preferential oxidation (COPROX), which is a promising process for the purification of hydrogen streams. In this work, we report a careful spectroscopic characterization of the said system, with the aim of relating its physical chemistry properties to the catalytic behavior. In all the Co-Mn —Ce samples, we detected the formation of partially developed (Mn,Co)_3O_4 mixed spinels. The presence of these species, which can be reduced during the TPR experiments at an intermediate temperature range (300-600 °C), was also suggested by XRD and LRS. XPS results show that in all cases the catalytic surface is enriched in Mn, while the opposite occurs for Co. As regards the catalytic activity, we observed that the best formulations were those containing intermediate Mn/Co ratios (1/4 and 1/1), which can be ascribed to the promoting effect of Mn in improving the redox properties of Co active sites and provoking an increase in surface area. The best catalyst, which has a Mn/Co ratio of 1/4, was very stable after 75 h of time-on-stream with CO_2 included in the feed.
机译:Mn-Co-Ce混合氧化物是CO优先氧化(COPROX)的活性和选择性催化剂,这是提纯氢气流的有前途的工艺。在这项工作中,我们报告了所述系统的仔细的光谱表征,目的是将其物理化学性质与催化行为联系起来。在所有的Co-Mn -Ce样品中,我们检测到部分显影的(Mn,Co)_3O_4混合尖晶石的形成。 XRD和LRS也暗示了这些物种的存在,在中间温度范围(300-600°C)的TPR实验中可以减少这些物种的存在。 XPS结果表明,在所有情况下,催化表面均富含Mn,而Co则相反。就催化活性而言,我们观察到最好的配方是那些具有中等Mn / Co比(1/4和1/1)的配方。 ),这可以归因于Mn在改善Co活性位点的氧化还原特性和引起表面积增加方面的促进作用。 Mn / Co比为1/4的最佳催化剂在运行75小时后非常稳定,进料中包含CO_2。

著录项

  • 来源
    《International journal of hydrogen energy》 |2013年第14期|5645-5654|共10页
  • 作者单位

    Institute de Investigaciones en Catdlisis y Petroquimica, INCAPE (FIQ UNL-CONICET), Santiago del Estero 2829, 3000 Santa Fe, Argentina;

    Institute de Investigaciones en Catdlisis y Petroquimica, INCAPE (FIQ UNL-CONICET), Santiago del Estero 2829, 3000 Santa Fe, Argentina;

    Institute de Investigaciones en Catdlisis y Petroquimica, INCAPE (FIQ UNL-CONICET), Santiago del Estero 2829, 3000 Santa Fe, Argentina;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Mn—Co—Ce mixed oxides; COPROX; XPS; raman; CO_2 tolerance; hydrogen;

    机译:Mn-Co-Ce混合氧化物;COPROX;XPS;拉曼;CO_2耐受性;氢;
  • 入库时间 2022-08-18 00:27:42

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