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Autothermal reforming of simulated and commercial fuels on zirconia-supported mono- and bimetallic noble metal catalysts

机译:氧化锆负载的单金属和双金属贵金属催化剂上模拟燃料和商用燃料的自动热重整

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摘要

New energy sources are needed if energy supply and demand are to remain in balance. At the same time, the level of emissions needs to be reduced to minimise their contribution to the greenhouse effect. Renewable energy sources, and hydrogen (H2), have been attracting much attention, and more efficient technologies for energy recovery have been developed. Among these are fuel cells. H2 is not a source of energy but an energy carrier, which needs to be produced from a primary fuel (hydrocarbons, alcohols, water). Conventionally H2 is produced by steam reforming (SR) of natural gas. For mobile applications, however, a liquid fuel that is easy to deliver and safe to store is at present more feasible. Since the reaction enthalpy of SR increases markedly with the length of the hydrocarbon chain of the fuel, autothermal reforming (ATR), where endothermic SR is combined with exothermic partial oxidation (POX), is preferable to conventional SR. ATR of hydrocarbon fuels was investigated for the on-site production of H2-rich fuel gas suitable for solid oxide fuel cell (SOFC) applications. ATR of commercial fuels has to be carried out at high temperatures (700–900 °C) to achieve complete conversion of both the aliphatic and aromatic hydrocarbon fractions. With high temperature, however, thermal reactions of aliphatic hydrocarbons accelerate producing undesired compounds that also promote coke formation. These challenges can be overcome with active, selective and stable catalysts. ZrO2-supported mono- and bimetallic noble metal (Rh, Pd, Pt) catalysts were examined. Rh proved to be most active for SR, whereas Pt was active for oxidation reactions. The good features of these two metals were combined in the bimetallic catalysts where strong synergism exists between Rh and Pt. Catalytic performance was excellent, there were no side products and coke formation was suppressed. Furthermore, ATR of commercial low-sulfur diesel was successfully carried out on these bimetallic RhPt catalysts, which exhibited high thermal stability even in the presence of heterocyclic sulfur compounds.
机译:如果要保持能源供需平衡,就需要新能源。同时,需要降低排放水平,以最大程度地减少其对温室效应的影响。可再生能源和氢气(H2)一直备受关注,并且已开发出更高效的能量回收技术。其中有燃料电池。 H2不是能源,而是能量载体,需要从主要燃料(碳氢化合物,酒精,水)中产生。常规地,H 2是通过天然气的蒸汽重整(SR)产生的。然而,对于移动应用而言,目前易于运输和安全存储的液体燃料更加可行。由于SR的反应焓随燃料烃链长度的增加而显着增加,因此吸热SR与放热部分氧化(POX)相结合的自热重整(ATR)比常规SR更好。为了现场生产适用于固体氧化物燃料电池(SOFC)的富含H2的燃料气体,对烃类燃料的ATR进行了研究。商业燃料的ATR必须在高温(700–900°C)下进行,以实现脂肪族和芳香族烃馏分的完全转化。然而,在高温下,脂族烃的热反应加速了产生不期望的化合物,这些化合物也促进了焦炭的形成。这些挑战可以通过活性,选择性和稳定的催化剂来克服。研究了ZrO2负载的单金属和双金属贵金属(Rh,Pd,Pt)催化剂。事实证明,Rh对SR最具活性,而Pt对氧化反应具有活性。在Rh和Pt之间存在很强的协同作用的双金​​属催化剂中,结合了这两种金属的优良特性。催化性能优异,没有副产物,并且抑制了焦炭形成。此外,在这些双金属RhPt催化剂上成功进行了商业低硫柴油的ATR,即使在存在杂环硫化合物的情况下,它们也显示出高的热稳定性。

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    Kaila Reetta;

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  • 年度 2008
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  • 原文格式 PDF
  • 正文语种 en
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