催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (12): 1483-1488.DOI: 10.3724/SP.J.1088.2010.00617

• 研究论文 • 上一篇    下一篇

钴基催化剂在费-托反应过程中的失活行为

石利红 1,2, 李晓峰 3, 李德宝 2, 孙予罕 2   

  1. 1 山西大学化学化工学院, 山西太原 030006; 2 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001; 3 太原幼儿师范学校基础理科, 山西太原 030027
  • 收稿日期:2010-06-11 出版日期:2010-12-13 发布日期:2014-04-26

Deactivation of Cobalt-Based Catalysts for Fischer-Tropsch Synthesis

SHI Lihong1,2,*, LI Xiaofeng3, LI Debao2, SUN Yuhan2   

  1. 1School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, Shanxi, China; 2State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 3Taiyuan Infant Normal School, Taiyuan 030027, Shanxi, China
  • Received:2010-06-11 Online:2010-12-13 Published:2014-04-26

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1037

被引次数

9

摘要： 考察了 Co/SiO2, Co/Ru/SiO2 和疏水改性 Co/Ru/SiO2 催化剂在费-托合成过程中的稳定性.结果发现, 随着反应的进行, 三种催化剂都呈现一定程度的失活,它们稳定性高低顺序为: 疏水改性 Co/Ru/SiO2 > Co/SiO2 > Co/Ru/SiO2. Co/SiO2 催化剂的失活是由于催化剂上 Co 晶粒的长大和硅酸钴物种的生成, 而 Co/Ru/SiO2和疏水改性 Co/Ru/SiO2的失活则是由于催化剂上 Co 晶粒的长大所致. 由于 Co/Ru/SiO2 催化剂的 Co 晶粒比 Co/SiO2催化剂的小得多, 在反应过程中更容易长大, 所以 Co/Ru/SiO2催化剂稳定性更差; 而疏水改性 Co/Ru/SiO2催化剂表面的疏水性既抑制了硅酸钴物种的形成, 又使 Co 晶粒长大较慢, 因此其稳定性最高.

关键词: 钴, 钌, 费-托合成, 疏水改性, 失活

Abstract: Stability tests of Co/SiO2, Co/Ru/SiO2, and hydrophobically-organically modified Co/Ru/SiO2 (Co/Ru/SiO2-S) for Fischer- Tropsch synthesis were carried out. As the time on stream went on, CO conversion decreased in all the cases. The growth of cobalt crystallite and the formation of cobalt silicates species were the reasons for Co/SiO2 deactivation, while the deactivation of Co/Ru/SiO2 and Co/Ru/SiO2-S was only attributed to the growth of cobalt crystallite. The stability of the catalysts was in order of Co/Ru/SiO2-S > Co/SiO2 > Co/Ru/SiO2. Compared with Co/SiO2, the faster deactivation rate for Co/Ru/SiO2 was ascribed to the agglomeration of smaller metal clusters, which were more unstable than the larger metal clusters and therefore more susceptible to sintering processes. Co/Ru/SiO2-S showed the best stability because of no formation of cobalt silicates species and the slow growth of cobalt crystallite.

Key words: cobalt, ruthenium, Fischer-Tropsch synthesis, hydrophobically-organic modification, deactivation