Vibrational Analysis of an Industrial Fe-Based Fischer-Tropsch Catalyst Employing Inelastic Neutron Scattering
Vibrational Analysis of an Industrial Fe-Based Fischer-Tropsch Catalyst Employing Inelastic Neutron Scattering
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采用非弹性中子散射对工业铁基费托催化剂进行振动分析
DOI：
10.1002/ange.201210179
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发表时间：
2013
影响因子：
--
通讯作者：
Hamilton N
中科院分区：
文献类型：
--
作者：
Hamilton N
在过去的几十年里，费托(FT)催化剂的研究活动再次活跃起来，用于将合成气(CO+H2)转化为汽油和柴油。[1]这种FT复兴恰逢最近世界各地几个工业装置投产。[2]尽管有这样的活性范围，FT催化剂的实际操作仍然存在一些不确定性。这一经济意义重大的反应系统的内在复杂性在舒尔茨оS的描述中得到了解释，FT催化剂的活性相是在自组织过程中在反应条件下构建的。[3]尽管新的FT单元操作倾向于以钴基催化剂为特色，但人们对铁基催化剂仍有相当大的兴趣。例如，Weckhuysen和他的同事使用理论和实验相结合的方法来监测铁基FT催化剂中的原位相变。[4]最近的研究表明，铁基FT催化剂如何能够比高分子量烷烃更有利于低分子烯烃的生产。[5]为了更好地了解Fe基FT催化剂的功能，我们研究了一种工业反应的Fe基FT催化剂，它使用非弹性中子散射(INS)作为主要的振动探针，因为它能够表征含氢物种。[6]有关催化剂回收方法的描述，请参阅实验部分。目前，X-射线衍射仪(XRD)、穆斯堡尔谱和程序升温氧化(TPO)等分析技术被用来从固态化学(磁铁矿+碳化铁)[7]和碳质材料的存在方面对铁FT催化剂进行表征。[8]这里使用的InS光谱仪(TOSCA)以前曾被用来探索用于CH4干法重整的工业相关镍催化剂中的碳氢物种。[9]然而，这项工作首次适用于INS，以考虑氢部分在Fe FT催化剂基质中的保留。Parker和他的同事们对INS在探索多相催化剂方面的应用进行了综述。
The last few decades have witnessed a resurgence of research activity into Fischer–Tropsch (FT) catalysis, for the conversion of syngas (CO+ H2) into gasoline and diesel.[1] This FT renaissance coincides with the recent commissioning of several industrial unit operations around the world.[2] Despite this range of activity, some uncertainties still remain about the actual operation of the FT catalyst. The inherent complexity of this economically highly significant reaction system is paraphrased in Schulzоs description of the active phase of a FT catalyst as being constructed under reaction conditions during a process of self-organization.[3] Although the new FT unit operations tend to feature Cobased catalysts, there remains considerable interest in Febased catalysts. For example, Weckhuysen and co-workers have used a combination of theory and experiment to monitor insitu phase changes in Fe-based FT catalysts.[4] More recently, studies have shown how iron-based FT catalysts can be adapted to favor the production of low-molecularweight olefins over high-molecular-weight alkanes.[5] To obtain a better understanding of the function of an Febased FT catalyst, we have studied an industrially reacted Febased FT catalyst using inelastic neutron scattering (INS) as the principal vibrational probe because of its ability to characterize hydrogen-containing species.[6] For a description of the catalyst recovery method, see the Experimental Section. Analytical techniques such as X-ray diffraction (XRD), Mçssbauer spectroscopy and temperature-programmed oxidation (TPO), are currently used to characterize iron FT catalysts with respect to solid-state chemistry (magnetite plus iron carbides)[7] and the presence of carbonaceous materials.[8] The INS spectrometer used here (TOSCA) has been used previously to probe hydrocarbonaceous species in an industrially relevant Ni catalyst used for the dry reforming of CH4.[9] However this work applies INS for the first time to consider the retention of hydrogenous moieties within the Fe FT catalyst matrix. The application of INS to probe heterogeneous catalysts has been reviewed by Parker and co-workers.[10]