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High stability of Ce-promoted Ni/Mg-Al catalysts derived from hydrotalcites in dry reforming of methane

机译：铈的水滑石衍生的铈促进Ni / Mg-Al催化剂在甲烷干重整中的高稳定性

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摘要

Ce-promoted Ni/Mg-Al catalysts were synthesized by means of a methodology that involves the doping of Ni-Mg-Al mixed oxides derived from hydrotalcites with [Ce(EDTA)]~- and subsequent thermal decomposition. The effect of the nominal load of Ce in the catalytic performance of the materials was studied. The solids were characterized by means of XRD, BET area, TPR-H_2, TPD-CO_2, chemical analysis by ICPs, TGA, SEM and TEM and were evaluated in CO_2 reforming of methane at 700 ℃. The results indicate the partial reconstruction of the periclase phase during the doping with [Ce(EDTA)]~- and the formation of a mixture of crystalline periclase and fluorite phases after the calcination. Catalysts with particle sizes of Ni° between 5 and 9 nm were obtained. Ce presents a promote effect in the degree of reduction of Ni and the amount and strength of the basic sites. It was evident a beneficial effect of cerium in the catalytic activity and selectivity of the doped materials. The increase of the nominal Ce load between 1 and 10% causes no considerable effect in the cataiytic activity and selectivity or in the size of crystallite in these materials but in the inhibition of the coke formation. The catalysts show excellent catalytic performance under drastic conditions of reaction and long operation times. The Ce-doped Ni/Mg-Al catalyst is stable up to 100 h of reaction using a feed mixture of CH_4/CO_2/He 10/10/80 at 24 L g~(-1) h~(-1), up to 20 h of reaction using CO_2/CH_4 20/20 at 48 L g~(-1) h~(-1) and up to 15 h of reaction using CO_2/CH_4 40/40 at 96 L g~(-1) h~(-1). The filamentous coke formation is demonstrated on the surface of the catalyst when gas of dilution in the reactants is not used. The developed method of synthesis becomes an interesting methodology for obtaining catalysts for CO_2 reforming of methane.
机译：Ce促进的Ni / Mg-Al催化剂是通过一种方法合成的，该方法涉及用[Ce（EDTA）]-掺杂水滑石衍生的Ni-Mg-Al混合氧化物，然后进行热分解。研究了铈标称载荷对材料催化性能的影响。通过XRD，BET面积，TPR-H_2，TPD-CO_2，ICPs，TGA，SEM和TEM等方法对固体进行表征，并在700℃下甲烷甲烷重整中进行了评价。结果表明，在掺杂[Ce（EDTA）]-的过程中，钙长石相部分重构，并且在煅烧后形成结晶的钙长石相和萤石相的混合物。获得具有5至9nm的Ni°粒径的催化剂。 Ce对Ni的还原度以及碱性部位的数量和强度具有促进作用。显然铈对掺杂材料的催化活性和选择性具有有益的作用。 Ce的名义负载量增加1％至10％不会对这些材料的催化活性和选择性或微晶尺寸产生重大影响，但会抑制焦炭的形成。在剧烈的反应条件下和长的操作时间下，该催化剂表现出优异的催化性能。使用CH_4 / CO_2 / He 10/10/80的进料混合物在24 L g〜（-1）h〜（-1）或更高的温度下，Ce掺杂的Ni / Mg-Al催化剂在100小时的反应中稳定。使用CO_2 / CH_4 20/20在48 L g〜（-1）h〜（-1）的条件下反应20小时，以及使用CO_2 / CH_4 40/40在96 L g〜（-1）的条件下长达15小时的反应h〜（-1）。当不使用在反应物中稀释的气体时，在催化剂表面上证明了丝状焦炭的形成。发达的合成方法成为获得甲烷CO_2重整催化剂的有趣方法。

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  • 来源
    《Fuel》 |2010年第3期|592-603|共12页
  • 作者

    Carlos Enrique Daza; Jaime Gallego; Fanor Mondragon; Sonia Moreno; Rafael Molina;

  • 作者单位

    Estado Solido y Catdlisis Ambiental, Departamento de Quimica, Facultad de Ciencias, Universidad National de Colombia, AK 30 No. 45-03, Bogota, Colombia;

    Quimica de Recursos Energeticos y Medio Ambiente, Institute de Quimica, Universidad de Antioquia, P.O. Box A.A. 1226, Medellin, Colombia;

    Quimica de Recursos Energeticos y Medio Ambiente, Institute de Quimica, Universidad de Antioquia, P.O. Box A.A. 1226, Medellin, Colombia;

    Estado Solido y Catdlisis Ambiental, Departamento de Quimica, Facultad de Ciencias, Universidad National de Colombia, AK 30 No. 45-03, Bogota, Colombia;

    Estado Solido y Catdlisis Ambiental, Departamento de Quimica, Facultad de Ciencias, Universidad National de Colombia, AK 30 No. 45-03, Bogota, Colombia;

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

    hydrotalcites; mixed oxide; Ce; methane; dry reforming;

    机译：水滑石;混合氧化物铈甲烷干重整;

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