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首页> 外文期刊>Energy & fuels >Reactivity of Oxygen Carriers for Chemical-Looping Combustion in Packed Bed Reactors under Pressurized Conditions
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Reactivity of Oxygen Carriers for Chemical-Looping Combustion in Packed Bed Reactors under Pressurized Conditions

机译：加压条件下填充床反应器中氧气载体对化学循环燃烧的反应性

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摘要

For the design, scale-up, and optimization of pressurized packed bed reactors for chemical-looping combustion (CLC), understanding of the effect of the pressure on the reactivity of the oxygen carriers is very important. In this work, the redox reactivity of CuO/Al2O3 and NiO/CaAl2O4 particles at elevated pressures have been measured in a pressurized high-temperature magnetic suspension balance. The experiments have demonstrated that the pressure has a negative influence on the reactivity and that this effect is kinetically controlled. The negative effect of the pressure might be caused by the decrease in the number of oxygen vacancies at higher pressures. Moreover, the reactant gas fraction has been demonstrated as an important parameter, probably related to competition between different species for adsorption on the oxygen carrier surface. These effects have been included in the kinetic model leading to a good description of the experimental results. The impact of these findings on packed bed CLC applications with larger oxygen carrier particles has been investigated with a particle model that considers diffusion limitations and kinetics. It has been shown that the impact of diffusion limitations decreases with increasing pressure, due to the decrease in reaction rates and the increase in diffusion fluxes caused by Knudsen diffusion. The results have been validated by experiments with 1.7 mm NiO/CaAl2O4 particles. These results corroborate that the selection of larger particles because of pressure drop considerations does not lead to a large decrease in effective reaction rates, which is beneficial for packed bed CLC applications.
机译：对于设计，放大和优化用于化学回路燃烧（CLC）的加压填充床反应器，了解压力对氧载体反应性的影响非常重要。在这项工作中，已经在加压的高温磁悬浮天平中测量了在高压下CuO / Al2O3和NiO / CaAl2O4颗粒的氧化还原反应性。实验表明，压力对反应性有负面影响，并且这种影响是动力学控制的。压力的负面影响可能是由于较高压力下的氧空位数量减少所致。而且，已证明反应气体分数是重要的参数，可能与不同物质之间在氧气载体表面上的吸附竞争有关。这些效应已包含在动力学模型中，从而可以很好地描述实验结果。已经使用考虑了扩散限制和动力学的颗粒模型研究了这些发现对具有较大氧气载体颗粒的填充床CLC应用的影响。已经表明，由于反应速率的降低和由克努森扩散引起的扩散通量的增加，扩散限制的影响随着压力的增加而减小。通过使用1.7 mm NiO / CaAl2O4颗粒进行的实验验证了结果。这些结果证实，由于考虑到压降而选择较大的颗粒不会导致有效反应速率大大降低，这对于填充床CLC应用是有利的。

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  • 来源
    《Energy & fuels》 |2015年第maraaapra期|2656-2663|共8页
  • 作者

    Hamers H. P.; Gallucci F.; Williams G.; Cobden P. D.; Annaland M. van Sint;

  • 作者单位

    Eindhoven Univ Technol, Dept Chem Engn & Chem, Chem Proc Intensificat, NL-5600 MB Eindhoven, Netherlands;

    Eindhoven Univ Technol, Dept Chem Engn & Chem, Chem Proc Intensificat, NL-5600 MB Eindhoven, Netherlands;

    Johnson Matthey Publ Ltd Co, Reading RG4 9NH, Berks, England;

    Energy Res Ctr Netherlands ECN, NL-1755 ZG Petten, Netherlands;

    Eindhoven Univ Technol, Dept Chem Engn & Chem, Chem Proc Intensificat, NL-5600 MB Eindhoven, Netherlands;

  • 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);
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