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Catalytic partial oxidation of methane over nickel and ruthenium based catalysts under low O-2/CH4 ratios and with addition of steam

机译:在低O-2 / CH4比率和添加蒸汽的情况下,镍和钌基催化剂上甲烷的催化部分氧化

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摘要

Catalytic partial oxidation (CPO) of methane to synthesis gas at low O-2/CH4 ratios and in the presence of steam was investigated over nickel and ruthenium catalysts supported on hydrotalcite-derived materials. The influence of catalyst properties and composition on activity, temperature profile and deactivation by carbon formation was examined. All catalyst presented high methane conversions, close to the values predicted by thermodynamic equilibrium and such conversions increased in proportion to the metal surface of the catalyst tested. The temperature profiles at O-2/CH4 = 0.2 and H2O/CH4 = 0.3 and a constant exit temperature of 700 degrees C varied depending on the catalyst type; it was possible to examine catalyst deactivation from the change in the shape of the profile of each catalyst. Since the O-2/CH4 and H2O/CH4 ratios were low, the risk or potential for carbon formation was thermodynamically favorable along the entire catalytic bed; however, this potential was qualitatively higher when the temperature profile of the catalyst presented a pronounced maximum peak at the inlet of the reactor. During catalytic reaction tests and methane decomposition experiments, the ruthenium catalyst did not formed appreciable amounts of carbon while a bimetallic catalyst (Ni and Ru) form only small amounts (in comparison with the nickel catalysts). For the ruthenium catalyst, a higher O-2/CH4 ratio favored conversions closer to the equilibrium value. The observations presented in this work indicate that during the CPO of methane, at low O-2/CH4 ratios and in the presence of steam, the catalyst properties and composition will have a substantial influence on the extent of the combustion and reforming reactions along the catalytic bed. This will in turn define the temperature profile, and therefore the risk or potential for carbon formation; this risk might effectively be overcome by the use of ruthenium-containing catalysts. (C) 2015 Elsevier Ltd. All rights reserved.
机译:在水滑石衍生材料上负载的镍和钌催化剂上,研究了低O-2 / CH4比例和在有蒸汽存在下甲烷到合成气的甲烷催化部分氧化(CPO)。考察了催化剂性能和组成对活性,温度曲线和碳形成失活的影响。所有催化剂均表现出高甲烷转化率,接近热力学平衡所预测的值,且此类转化率与所测试催化剂的金属表面成比例增加。 O-2 / CH4 = 0.2和H2O / CH4 = 0.3时的温度曲线以及700摄氏度的恒定出口温度取决于催化剂类型。可以根据每种催化剂的轮廓形状的变化来检查催化剂的失活。由于O-2 / CH4和H2O / CH4的比率低,因此在整个催化床中,形成碳的风险或潜力在热力学上是有利的。然而,当催化剂的温度曲线在反应器入口处出现明显的最大峰时,该电位在质量上更高。在催化反应测试和甲烷分解实验中,钌催化剂未形成可观数量的碳,而双金属催化剂(Ni和Ru)仅形成少量(与镍催化剂相比)。对于钌催化剂,较高的O-2 / CH4比值有利于转化率接近平衡值。这项工作中提出的观察结果表明,在甲烷CPO期间,在低O-2 / CH4比和存在蒸汽的情况下,催化剂的性质和组成将对沿甲烷燃烧和重整反应的程度产生重大影响。催化床。反过来,这将定义温度曲线,从而定义碳形成的风险或潜力;通过使用含钌催化剂可以有效地克服这种风险。 (C)2015 Elsevier Ltd.保留所有权利。

著录项

  • 来源
    《Fuel》 |2015年第1期|192-201|共10页
  • 作者单位

    KTH Royal Inst Technol, Sch Chem Sci & Engn, Chem Technol, SE-10044 Stockholm, Sweden|UMSA, Inst Gas Nat, La Paz, Bolivia;

    UMSA, Inst Gas Nat, La Paz, Bolivia;

    KTH Royal Inst Technol, Sch Chem Sci & Engn, Chem Technol, SE-10044 Stockholm, Sweden|UMSA, Inst Gas Nat, La Paz, Bolivia;

    UMSA, Inst Gas Nat, La Paz, Bolivia;

    KTH Royal Inst Technol, Sch Chem Sci & Engn, Chem Technol, SE-10044 Stockholm, Sweden;

    KTH Royal Inst Technol, Sch Chem Sci & Engn, Chem Technol, SE-10044 Stockholm, Sweden;

  • 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

    Carbon formation; Nickel; Partial oxidation of methane; Ruthenium; Synthesis gas;

    机译:碳形成;镍;甲烷部分氧化;钌;合成气;

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