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沉淀铁催化剂在F-T合成反应过程中的物相变化
Phase Change of Precipitated Iron Catalyst during Reaction Process of Fischer-Tropsch Synthesis
【摘要】 采用元素分析、X射线衍射和穆斯堡尔谱等手段研究了喷雾干燥沉淀Fe Cu K/SiO2 催化剂在F T合成反应过程中的物相变化 .结果表明 ,新鲜催化剂样品主要由α Fe2 O3 组成 ,且 81 1%的α Fe2 O3 粒径小于 13 5nm .随着反应时间的延长 ,催化剂表面碳沉积物的含量逐渐增多 ,不饱和度逐渐增大 ;χ Fe5C2 的含量逐渐增多 ,Fe3 O4的含量逐渐减少并趋于稳定 .超顺磁Fe3 + 的含量呈先增加后减少的变化趋势 .由于碳沉积物是由CO生成的 ,而 χ Fe5C2 是由α Fe2 O3 经Fe3 O4生成的 ,故催化剂表面碳沉积物的生成先于 χ Fe5C2 的生成 .
【Abstract】 The phase composition of spray dry precipitated Fe-Cu-K/SiO 2 catalyst for F-T synthesis was characterized by element analysis, X-ray diffraction and Mssbauer spectroscopy. The content of insoluble carbonaceous deposit and the C/H mole ratio on the catalyst surface increased with the time on stream. α-Fe 2O 3 was found in the fresh catalyst, and α-Fe 2O 3, Fe 3O 4 and χ-Fe 5C 2 were found in the catalyst samples after reaction for 19 and 451 h, respectively. With the increase of time on stream, the content of χ-Fe 5C 2 gradually increased, and the amount of Fe 3O 4 decreased nearly to stability; the content of Fe 3+ in a superparamagnetic state increased first, and then decreased. The formation of insoluble carbonaceous deposit was prior to that of χ-Fe 5C 2 owing to carbonaceous deposit from CO and χ-Fe 5C 2 from α-Fe 2O 3 via Fe 3O 4.
【Key words】 Fischer-Tropsch synthesis; iron; copper; potassium; silica; carbonaceous deposit; iron carbide;
- 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2004年05期
- 【分类号】O643
- 【被引频次】8
- 【下载频次】236