催化学报 ›› 2011, Vol. 32 ›› Issue (6): 1027-1034.DOI: 10.3724/SP.J.1088.2011.10116

• 研究论文 • 上一篇    下一篇

等离子体法制备钴基费-托合成催化剂及性能表征

黄承都, 白素丽, 吕静, 李振花*   

  1. 天津大学化工学院, 绿色合成与转化教育部重点实验室, 天津 300072
  • 收稿日期:2011-01-10 修回日期:2011-03-01 出版日期:2011-06-21 发布日期:2014-10-31

Preparation and Characterization of Co-Based Catalyst via Dielectric-Barrier Discharge Plasma Decomposition for Fischer-Tropsch Synthesis

HUANG Chengdu, BAI Suli, Lü Jing, LI Zhenhua*   

  1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  • Received:2011-01-10 Revised:2011-03-01 Online:2011-06-21 Published:2014-10-31

摘要: 钴基费-托合成催化剂以介质阻挡放电等离子体 (DBD法) 替代传统热焙烧过程来制备, 从而可在低温分解前驱体以获得高分散催化剂. 结果表明, DBD 法分解前驱体效果与传统焙烧法相同, 但更节能和快捷. 尽管两种方法所得催化剂的比表面积相近, 但 DBD 法制得催化剂的孔体积和孔径更大, Co 分散度更高, 且 Co 与载体间的相互作用更强, 因而更难还原. 同时, DBD 法处理催化剂时硝酸钴分解产物以 Co3O4 为主, 其粒径较小 (达 11.8 nm), 其团簇在催化剂表面分布比较均匀. 因此, 在费-托合成反应中 DBD 法制得的催化剂表现出较高的 CO 转化率和 C5+选择性.

关键词: 等离子体处理, 钴基催化剂, 介质阻挡放电, 前驱体分解, 费-托合成

Abstract: To obtain a highly dispersed Co-based catalyst, dielectric-barrier discharge (DBD) plasma instead of calcination was used to decompose the precursors at low temperature. It was found that DBD plasma can not only replace calcination to get catalyst precursor decomposed but also be quicker and more energy-saving. The catalyst samples treated by the two methods had similar surface area, while pore volume and pore size of the sample treated by DBD was larger than that by calcination. Temperature-programmed reduction results showed that the catalyst treated by DBD resulted in higher Co dispersion and stronger interaction between Co and the support than that by calcination. X-ray diffraction results indicated that Co3O4 was the main Co species after DBD treatment. The Co3O4 crystallite diameter was 11.8 nm, which was smaller than that of calcined counterparts. Transmission electron microscopy results proved that DBD treatment resulted in smaller Co oxide clusters, more homogeneous Co distribution, and less agglomeration. Fischer-Tropsch synthesis performance evaluation results showed that DBD treated catalyst had higher CO conversion and C5+ selectivity than the calcined one.

Key words: plasma treatment, Co-based catalyst, dielectric-barrier discharge, precursor decomposition, Fischer-Tropsch synthesis