化学学报 ›› 2008, Vol. 66 ›› Issue (16): 1851-1856.    下一篇

研究论文

介孔氧化硅球负载钴基催化剂在费托合成中的应用

高 恋a,b 徐 耀*,a 侯 博a 吴 东a 孙予罕*,a

  

  1. (a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)
    (b中国科学院研究生院 北京 100039)

  • 收稿日期:2008-01-07 修回日期:2008-03-31 出版日期:2008-08-28 发布日期:2008-08-28
  • 通讯作者: 徐耀

Application of Hollow Mesoporous Silica Sphere Supported Cobalt Catalysts in Fischer-Tropsch Synthesis

GAO, Lian a,b XU, Yao *,a HOU, Bo a WU, Dong a SUN, Yu-Han *,a   

  1. (a State Key Laboratory of Coal Conversion, Shanxi Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001)
    (b Graduate University of the Chinese Academy of Sciences, Beijing 100039)
  • Received:2008-01-07 Revised:2008-03-31 Online:2008-08-28 Published:2008-08-28
  • Contact: XU, Yao

以介孔氧化硅空心球(HMSS)为载体, 采用双溶剂法浸渍硝酸钴溶液制备了高分散度的钴催化剂, 并表征了催化剂中Co3O4颗粒的负载情况和费托(F-T)反应性能. 结果表明: Co3O4颗粒在介孔硅球孔道内形成100~200 nm左右分散良好的簇团, 将催化剂压碎和刻蚀后的透射电子显微镜(TEM)证实, 这些簇团是由尺寸约为10~15 nm大小均匀的Co3O4单分散颗粒组成, 这些单分散颗粒锚定在介孔硅球孔道内, 彼此之间被相邻孔壁隔开; 催化剂中钴-硅作用很弱, 在600 K下即可被还原; F-T反应评价表明, 所得产物保持了良好的烃分布, 主要集中于C5~C18烃, 选择性在60%左右, C5+选择性达到80%以上.

关键词: 中空球, 双溶剂, F-T合成

High dispersion Co3O4 nano-particles supported on hollow mesoporous silica spheres (HMSS) were prepared by a novel two-solvent method. The supported nano-particles had been characterized and its catalytic performance had been evaluated. The Co3O4 single clusters were 100~200 nm and dispersed equably in the pore channels. HRTEM and TEM results showed that these single clusters were composed by 10~15 nm mono-dispersed Co3O4 nano-particles, and these Co3O4 nano-particles were loaded in the pore channels of the HMMS and were divided by the pore walls with each other. XRD and Raman spectra proved that the Co species in the catalysts were Co3O4 phase. The interaction between Co atom and Si atom was negligible, indicating that there was almost no Co2SiO3 in the catalysts and thus the samples were easily to be reduced. The catalysts have good performance and hydrocarbon distribution which concentrated on C5~C18 in F-T synthesis, C5+ content could be above 80%.

Key words: hollow mesoporous silica spheres (HMSS), two-solvent, Fischer-Tropsch synthesis