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A promising preparation method for highly active cobalt based Fischer-Tropsch catalysts supported on stabilized Al2O3

机译:稳定Al2O3负载基于高活性钴基托催化剂的有希望的制备方法

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The effectiveness of the addition of diethylene glycol (DEG) to the impregnating solution in synthesizing highly dispersed Co-based catalysts supported on stabilized alumina (Al2O3(s)) is investigated. Both the properties and catalytic performance in the Fischer-Tropsch synthesis (FTS) of the material obtained using DEG (CoDEG/Al2O3(s)) are compared with those of a catalyst with the same formulation but prepared without the addition of DEG in the impregnating solution (Co/Al2O3(s)). When using Co-nitrate as Co-precursor, the addition of DEG leads to a very fast and exothermic decomposition of Co-nitrate into Co oxides during the calcination step. This prevents the agglomeration of Co3O4 particles, thus generating highly dispersed Co3O4 crystallites on the support. In line with the decrease of the Co3O4 crystallites size, the CoDEG/Al2O3(s) catalyst is more difficult to reduce than the Co/Al2O3(s) catalyst. As a result, the metallic surface of the two catalysts is very similar. Nonetheless, when tested in the FTS, the CoDEG/Al2O3(s) catalyst shows CO conversion higher than the Co/Al2O3(s) sample. This is attributed to the high intrinsic activity (i.e. high Turnover Frequency, TOF) of the small Co crystallites of the CoDEG/Al2O3(s) catalyst. We explain this result assuming that the combustion phenomenon occurring during the fast calcination induced by the presence of DEG may generate structural defects on the catalyst surface that are beneficial for the FTS. Notably, the product distribution of CoDEG/Al2O3(s) catalyst is only slightly affected.
机译:研究了在合成稳定的氧化铝(Al 2 O 3)上负载的高度分散的Co基催化剂中合成高度分散的Co基催化剂的浸渍溶液的有效性。使用DEG获得的材料的性质和催化性能(CODEG / Al 2 O 3)与具有相同配方的催化剂的物质(Codeg / Al 2 O 3)进行比较但制备而不在浸渍中添加含量溶液(CO / AL2O3)。当使用共硝酸盐作为共前体时,在煅烧步骤期间加入DEG将含量非常快速,放热分解在煅烧过程中的共氧化物中。这防止了CO 3 O 4颗粒的凝聚,从而在载体上产生高度分散的CO3O4微晶。根据CO3O4微晶尺寸的降低,Codeg / Al 2 O 3催化剂比CO / Al 2 O 3(S)催化剂更难以减少。结果,两种催化剂的金属表面非常相似。尽管如此,当在FTS中测试时,Codeg / Al 2 O 3催化剂显示CO转化比CO / Al 2 O 3样品高。这归因于Codeg / Al 2 O 3催化剂的小Co微晶的高固有活性(即高周转频率,TOF)。我们解释了该结果,假设在通过DEG的存在诱导的快速煅烧期间发生的燃烧现象可以在对FTS有益的催化剂表面上产生结构缺陷。值得注意的是,Codeg / Al 2 O 3催化剂的产物分布仅略微影响。

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