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Hydrogen production by steam reforming of ethanol over nickel supported on La-modified alumina catalysts prepared by sol-gel

机译：通过溶胶-凝胶法制备的La改性氧化铝催化剂上负载的镍上的乙醇进行水蒸气重整制氢

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摘要

The catalytic properties for steam reforming of ethanol (SRE) of 10 wt.% nickel supported on La-modified alumina prepared by sol-gel were studied. Lanthanum oxide content was in the range 0-12 wt.%. Supports were calcined at 650 ℃ and catalysts were calcined at 450 ℃ and reduced at 600 ℃. Catalysts were characterized by ICP, XRD, TPR, TPO and TEM. The progressive La-addition to the support had several effects: a structural effect in the alumina, promotion of a better dispersion of the NiO phase and increased number of NiO species reducing at lower temperature. Average Ni crystal size as determined by XRD in reduced samples was 6.3 nm. The SRE at molar ratio H_2O/EtOH = 3 was studied and ethanol conversion as a function of temperature showed small differences as a function of the lanthanum content, but the hydrogen yield was much more important for La-containing catalysts. Deactivation experiments at 500 ℃ showed that catalysts with higher La content were more stable and that the strong decrease in the ethanol conversion occurred in the first hours on stream at these experimental conditions. A good correlation between deactivation trend, ethylene evolution and occurrence of lower temperature gasified carbon-type residues was established with the support composition. Sintering of Ni particles occurred in all samples after reaction, but despite the presence of larger Ni particles in the Ni/Al_2O_3-Lal 2 catalyst this was the most stable one. As lanthanum species are progressively present in the support its contribution to stabilization of the catalyst is certainly related to the enhancement of gasification of carbon residues on the surface of the catalyst but also to a close interaction with nickel particles.
机译：研究了用溶胶-凝胶法制备的负载在La改性氧化铝上的10％（重量）镍镍对乙醇（SRE）蒸汽重整的催化性能。氧化镧含量为0-12重量％。将载体在650℃下煅烧，将催化剂在450℃下煅烧并在600℃下还原。通过ICP，XRD，TPR，TPO和TEM对催化剂进行了表征。逐步向载体中添加La具有几种作用：氧化铝中的结构作用，促进更好地分散NiO相以及在低温下增加NiO种类的减少。通过XRD在还原样品中测定的平均Ni晶体尺寸为6.3nm。研究了摩尔比为H_2O / EtOH = 3时的SRE，乙醇转化率随温度的变化显示出随镧含量变化的小差异，但氢含量对于含La的催化剂更为重要。在500℃下的失活实验表明，在这些实验条件下，La含量较高的催化剂更稳定，乙醇转化率的下降很大。用该载体组合物建立了失活趋势，乙烯释放与较低温度气化的碳型残渣的发生之间的良好相关性。反应后所有样品中均发生了Ni颗粒的烧结，但是尽管Ni / Al_2O_3-Lal 2催化剂中存在较大的Ni颗粒，但这是最稳定的。由于镧物种逐渐存在于载体中，因此其对催化剂稳定的贡献当然与增强催化剂表面上的碳残留物的气化作用以及与镍颗粒的紧密相互作用有关。

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  • 来源
    《Fuel》 |2013年第5期|828-835|共8页
  • 作者

    C. Melchor-Hernandez; A. Gomez-Cortes; G. Diaz;

  • 作者单位

    Instituto de Fisica, Universidad National Autonoma de Mexico, Circuito de la Investigation Cientifica s, Cd. Universitaria, Mexico, DF 04510, Mexico;

    Instituto de Fisica, Universidad National Autonoma de Mexico, Circuito de la Investigation Cientifica s, Cd. Universitaria, Mexico, DF 04510, Mexico;

    Instituto de Fisica, Universidad National Autonoma de Mexico, Circuito de la Investigation Cientifica s, Cd. Universitaria, Mexico, DF 04510, Mexico;

  • 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

    hydrogen; ethanol; lanthana-alumina; nickel; sol-gel;

    机译：氢;乙醇镧-氧化铝;镍;溶胶凝胶;

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