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Examining the temporal behavior of the hydrocarbonaceous overlayer on an iron based Fischer–Tropsch catalyst

机译:检查烃类覆盖物在铁基费氏杂菌催化剂上的时间行为

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In order to examine fundamental processes connected with the use of an unpromoted iron based Fischer–Tropsch synthesis (FTS) catalyst, model studies examining the temporal formation of hydrocarbonaceous species that form over the catalyst are undertaken using a combination of temperature-programmed oxidation, powder X-ray diffraction, Raman scattering, transmission electron microscopy and inelastic neutron scattering (INS). Catalyst samples were exposed to ambient pressure CO hydrogenation at 623 K for defined periods of time-on-stream (3, 6, 12 and 24 h) prior to analysis. INS reveals a progressive retention of hydrogenous species that is associated with the evolution of a hydrocarbonaceous overlayer, as evidenced by the presence of sp ~(2) and sp ~(3) hybridized C–H vibrational modes. Correlations between the formation of aliphatic and olefinic/aromatic moieties with post-reaction characterization leads to the proposal of a number of chemical transformations that, collectively, define the conditioning phase of the catalyst under the specified set of reaction conditions. A comparison between the inelastic neutron scattering spectra of the 24 h sample with that of an iron catalyst extracted from a commercial grade Fischer–Tropsch reactor validates the relevance of the experimental approach adopted.
机译:为了检查与使用非突出的铁基的费 - 托合成(FTS)催化剂连接的基本过程,使用温度编程氧化,粉末的组合来检查形成在催化剂上形成的烃类物种的时间形成的模型研究X射线衍射,拉曼散射,透射电子显微镜和无弹性中子散射(INS)。在分析之前,在623K下暴露于623k的环境压力CO氢化的环境压力CO氢化。 INS揭示了与烃类覆盖器的换档相关的易腐蚀性物质,如SP〜(2)和SP〜(3)杂交的C-H振动模式的存在所证明。脂族和烯烃/芳香部分的形成与反应后表征的相关性导致许多化学转化的提议,其在规定的反应条件下统称地限定催化剂的调理相。 24小时样品的非弹性中子散射光谱与从商业级Fischer-Tropsch反应器中提取的铁催化剂的非弹性中子散射光谱验证了所采用的实验方法的相关性。

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