助剂对铁基费托合成催化剂氧化行为的影响:H2O作用的解读

Effect of the promoters on oxidation behavior of Fe-based Fischer-Tropsch catalyst: Deciphering the role of H2O

  • 摘要: 以纯Fe催化剂为研究对象,采用XRD、Raman和TPH等手段考察了催化剂的碳化程度、还原程度对H2O氧化过程的影响,获得了H2O氧化过程与催化剂中碳物种转变之间的相互影响规律;系统考察了典型的费托合成助剂K和SiO2存在时对催化剂物化性质以及H2O氧化行为的影响,发现催化剂的碳化程度越高,碳化铁的抗H2O氧化能力越强,氧化过程使得碳物种的石墨化程度增加。适量K助剂可促进碳化铁和催化剂表面石墨碳的形成,提高了碳化铁在H2O氧化过程中的稳定性;SiO2助剂的加入显著抑制了催化剂的碳化,但可有效提高碳化铁以及碳物种的稳定性。

     

    Abstract: The effect of carburization and reduction degree on H2O oxidation behaviour for the iron carbides in Fe-based FTS catalyst were firstly investigated using a combination method including X-ray diffraction (XRD), Raman and temperature-programmed-hydrogenation (TPH). The relationship between carbon species transformation and H2O oxidation behaviour of iron carbides was investigated simultaneously. Based on these observations, the influence of typical promoters like K and SiO2 on the structure and H2O oxidation behaviour of Fe-based FTS catalysts was further studied. The results indicated that, for the iron catalyst, the stability of iron carbides against H2O oxidation was increased with the increase of iron carbides content, and the H2O oxidation process led to the formation of more graphitic carbon. The carburization ability was effectively enhanced when certain amount of K promoter was incorporated. Addition of K into Fe-based FTS catalyst increased the number of graphitic carbons, which increased the stability of iron carbides toward H2O oxidation ultimately. It was also found that promotion of SiO2 greatly degraded the carburization degree of the catalyst, while their tendency to be oxidized to form Fe3O4 in the H2O atmosphere was obviously hindered.

     

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