催化学报 ›› 2011, Vol. 32 ›› Issue (2): 368-373.DOI: 10.3724/SP.J.1088.2011.01003

• 研究论文 • 上一篇    下一篇

制备方法对双介孔钴基催化剂结构及其费-托反应性能的影响

王俊刚 1,2, 李德宝 1, 侯博 1, 贾丽涛 1, 贾利宏 1,2, 孙志强 3, 刘斌 3, 郭金刚 4, 任润厚 4, 孙予罕 1,5   

  1. 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, 山西太原 030001; 2中国科学院研究生院, 北京 100049; 3山西潞安煤基合成油有限公司, 山西屯留 046100; 4潞安 (矿业) 集团有限公司, 山西长治 046204; 5中国科学院上海高等研究院, 上海 201203
  • 收稿日期:2010-10-06 修回日期:2010-11-22 出版日期:2011-01-26 发布日期:2014-06-25

Influence of Preparation Methods on Catalytic Performance of Double Mesoporous Co-Based Catalysts for Fischer-Tropsch Synthesis

WANG Jungang1,2, LI Debao1,*, HOU Bo1, JIA Litao1 , JIA Lihong1,2, SUN Zhiqiang3, LIU Bin3, GUO Jingang4, REN Runhou4, SUN Yuhan1,5,*   

  1. 1State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China;  2Graduate University of Chinese Academy of Sciences, Beijing 100049, China;  3Lu’an Coal to Synfuel Co. Ltd, Tunliu 046100, Shanxi, China;  4Shanxi Lu’an (Mining) Group Co. Ltd, Changzhi, 046204, Shanxi, China;  5Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shangha, 201203, China
  • Received:2010-10-06 Revised:2010-11-22 Online:2011-01-26 Published:2014-06-25

摘要: 以双介孔分布 MCM-41 分子筛为载体, 采用等体积浸渍、氨水气相诱导水解和过量浸渍法制备了费-托合成钴基催化剂, 并考察了它们的孔结构、活性物种分布及费-托合成催化性能. 结果表明, 采用等体积浸渍法和氨水气相诱导水解法制备的催化剂都保持了较好的双介孔特性, Co 颗粒大部分位于分子筛的孔道内部. 过量浸渍法和等体积浸渍法制备的催化剂上 Co 物种的还原度和分散度均较高, 尤其后者上 Co 分散度更高, 因而具有较低的 CH4 选择性和较高的 C5+选择性.

关键词: 双介孔, MCM-41 分子筛, 制备方法, 钴基催化剂, 费-托合成

Abstract: A series of cobalt-based catalyst samples supported on double mesoporous MCM-41 for Fischer-Tropsch synthesis (FTS) were prepared using three methods, incipient-wetness impregnation (IWI), vapor-induced hydrolysis (VIH), and excessive impregnation (EI). The catalyst samples were characterized by N2 physisorption, X-ray diffraction (XRD), temperature-programmed reduction (H2-TPR) and Raman spectroscopy. The N2 physisorption results showed that the samples prepared by IWI and VIH retained the double mesoporous character, and the cobalt particles were mainly located in the pore. The FTS results showed that the reducibility and dispersion of active species of the samples prepared by IWI and EI were very high. The catalyst prepared by IWI had the smallest Co3O4 crystallite size and the highest dispersion and showed higher FTS activity, lower CH4 selectivity and higher C5+ selectivity.

Key words: double mesoporous, MCM-41 zeolite, preparation method, cobalt-based catalyst, Fischer-Tropsch synthesis