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The use of La_(1_x)Sr_xFeO_3 perovskite-type oxides as oxygen carriers in chemical-looping reforming of methane

机译:La_(1_x)Sr_xFeO_3钙钛矿型氧化物在甲烷化学循环重整中作为氧载体的用途

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摘要

La_(1_x)Sr_xFeO_3 perovskite-type oxides with x = 0.1, 0.3, 0.5, and 0.9 were prepared by combustion method. The synthesized perovskites were characterized by means of X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) surface area, temperature-programmed reduction (TPR), and Fourier transformed infrared spectroscopy (FTIR). Pure phase of perovskite-type crystalline structure was obtained regardless of the degree of Sr substitution. TPR, FTIR, and XRD results suggests that the electronic unbalance caused by the partial substitution for La~(3+) by Sr~(2+) is compensated by oxidation of a fraction of Fe~(3+) to Fe~(4+) and/or generation of oxygen vacancies in the perovskite lattice. There exist two kinds of oxygen species on the oxides: surface absorption oxygen and bulk lattice oxygen. The surface oxygen contributed to oxidize methane completely to CO_2 and H_2O because of its higher reactivity, while the other one prone to methane partial oxidation into H_2 and CO. The activity of the substituted perovskites decreases as the degree of substitution x > 0.5. However, Sr substitution would inhibit methane decomposition in the methane reaction with La_(1_x)Sr_xFeO_3 perovskites. An optimal range of the degree of Sr substitution is x = 0.3-0.5 for La_(1_x)Sr_xFeO_3. The multicyclic redox reaction results indicated that the synthesized perovskite-type oxides have good regenerability, which is a very important performance required in chemical-looping reforming of methane.
机译:通过燃烧法制备x = 0.1、0.3、0.5和0.9的La_(1_x)Sr_xFeO_3钙钛矿型氧化物。合成的钙钛矿通过X射线衍射(XRD),扫描电子显微镜(SEM),Brunauer-Emmett-Teller(BET)表面积,程序升温还原(TPR)和傅里叶变换红外光谱(FTIR)进行表征。无论Sr取代的程度如何,都获得钙钛矿型晶体结构的纯相。 TPR,FTIR和XRD结果表明,由Sr〜(2+)部分取代La〜(3+)引起的电子不平衡可通过一部分Fe〜(3+)氧化为Fe〜(4)来补偿。 +)和/或在钙钛矿晶格中产生氧空位。氧化物上存在两种氧:表面吸收氧和体晶格氧。表面氧由于其较高的反应性而将甲烷完全氧化为CO_2和H_2O,而另一种则易于将甲烷部分氧化为H_2和CO。取代的钙钛矿的活性随取代度x> 0.5的降低而降低。但是,Sr取代会抑制与La_(1_x)Sr_xFeO_3钙钛矿的甲烷反应中的甲烷分解。对于La_(1_x)Sr_xFeO_3,Sr取代度的最佳范围是x = 0.3-0.5。多环氧化还原反应结果表明,合成的钙钛矿型氧化物具有良好的可再生性,这是甲烷化学循环重整所需的非常重要的性能。

著录项

  • 来源
    《Fuel》 |2013年第6期|465-473|共9页
  • 作者单位

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

    The Key Laboratory of Renewable Energy and Gas Hydrate of Chinese Academy of Sciences, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;

  • 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

    synthesis gas; chemical-looping reforming; La_(1_x)Sr_xFeO_3 perovskites; oxygen carrier; methane;

    机译:合成气化学循环重整;La_(1_x)Sr_xFeO_3钙钛矿;氧气载体甲烷;

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