物理化学学报 >> 2007, Vol. 23 >> Issue (08): 1151-1156.doi: 10.1016/S1872-1508(07)60059-X

研究论文 上一篇    下一篇

F-T合成Fe/Cu/K/Al2O3催化剂的结构性质、还原及碳化行为

万海军; 吴宝山; 安霞; 陶智超; 李廷真; 相宏伟; 李永旺   

  1. 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 太原 030001; 中国科学院研究生院, 北京 100049
  • 收稿日期:2007-01-31 修回日期:2007-04-13 发布日期:2007-08-03
  • 通讯作者: 吴宝山 E-mail:wbs@sxicc.ac.cn

Structural Properties, Reduction and Carburization Behaviors of Fe/Cu/K/Al2O3 Catalyst for Fischer-Tropsch Synthesis

WAN Hai-Jun; WU Bao-Shan; AN Xia; TAO Zhi-Chao; LI Ting-Zhen; XIANG Hong-Wei; LI Yong-Wang   

  1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China; Graduate University of the Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2007-01-31 Revised:2007-04-13 Published:2007-08-03
  • Contact: WU Bao-Shan E-mail:wbs@sxicc.ac.cn

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摘要： 采用连续共沉淀与喷雾干燥成型技术相结合的方法制备了微球状Fe/Cu/K/Al2O3催化剂, 结合TG、N2物理吸附、XRD、H2-TPR、CO-TPR、Mossbauer谱等表征手段, 研究焙烧温度对Fischer-Tropshc (F-T)合成铁基催化剂的结构性质、还原行为和碳化行为的影响. 结果表明, 较高的焙烧温度有利于碳酸盐的分解和结晶水的脱除, 促进了催化剂的还原. 随着焙烧温度的进一步升高, 催化剂的比表面积减小, 平均孔径增大, α-Fe2O3晶粒的粒径增大, 催化剂中金属与载体的相互作用增强, 从而削弱了CuO、K2O助剂的作用, 严重抑制了催化剂的还原和碳化.

关键词: F-T合成, 铁基催化剂, 焙烧温度, 结构性质, 还原行为, 碳化行为

Abstract: An Fe/Cu/K/Al2O3 catalyst for Fischer-Tropsch synthesis (FTS) was prepared by using a combination of co-precipitation and spray-drying method. Thermal gravity (TG), N2 physisorption, X-ray diffraction (XRD), H2 temperature programmed reduction (H2-TPR), CO temperature programmed reduction (CO-TPR), and Mossbauer effect spectroscopy (MES), were used to investigate the effects of different calcination temperatures on the structural properties, reduction, and carburization behaviors of the iron-based catalyst. The results indicated that an increase in calcination temperature facilitated the carbonate decomposition and H2O removal and promoted the reduction of the catalyst. With further increasing the calcination temperature, the BET surface area of the catalyst decreased, and the size of the catalyst crystallite and the average pore diameter increased. Furthermore, high calcination temperature enhanced the metal-support interaction, which weakened the promotional effect of CuO and K2O, and therefore, severely suppresseed the reduction and carburization behaviors of the catalyst.

Key words: Fischer-Tropsch synthesis, Iron-based catalyst, Calcination temperature, Structural properties, Reduction behavior, Carburization behavior