催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (8): 681-686.

• 研究论文 • 上一篇    下一篇

SO2-4对铁基催化剂上费托合成反应的影响

安霞1,2,吴宝山1,万海军1,2,李廷真1,2,陶智超1,2,相宏伟1,李永旺1   

  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
  • 收稿日期:2007-08-25 出版日期:2007-08-25 发布日期:2011-08-19

Effect of SO2-4 on Fischer-Tropsch Synthesis over Iron-Based Catalyst

AN Xia1,2, WU Baoshan1*, WAN Haijun1,2, LI Tingzhen1,2, TAO Zhichao1,2, XIANG Hongwei1, LI Yongwang1   

  1. 1 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 2 Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2007-08-25 Online:2007-08-25 Published:2011-08-19

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769

被引次数

5

摘要： 以FeCuK/SiO2为母体催化剂,用不同浓度的NH4HSO4水溶液进行等体积浸渍,制备了不同SO2-4含量的费托合成(FTS)铁基催化剂. 采用原子发射光谱、低温N2吸附、X射线光电子能谱、程序升温还原和穆斯堡尔谱等技术对催化剂进行了表征,并在H2/CO摩尔比0.67, WHSV=2000h-1, 压力1.5 MPa和温度250 ℃条件下进行了浆态床FTS反应. 结果表明,少量SO2-4能促进催化剂在H2中的还原; 在合成气还原过程中,少量SO2-4对催化剂的碳化程度影响不大,但大量SO2-4严重抑制催化剂的碳化. 在约500 h的运行实验中,各催化剂样品表现出的催化活性有所差异,但均呈现较好的稳定性. SO2-4可抑制水煤气变换反应活性,且随着SO2-4含量的增加,抑制作用愈加明显; 同时,催化剂上浸渍少量SO2-4可有效抑制CH4的生成,提高低碳烯烃的选择性.

关键词: 硫酸根, 费托合成, 铁基催化剂, 浆态床反应器

Abstract: A series of Fe-based catalyst samples with different amounts of SO2-4 for Fischer-Tropsch synthesis (FTS) were prepared by iso-volume impregnation of the FeCuK/SiO2 precursor with NH4HSO4 solution. The catalyst samples were characterized by atomic emission spectroscopy, N2 adsorption,X-rayphotoelectron spectroscopy, temperature-programmed reduction, and Mssbauer effect spectroscopy. The catalytic performance of the catalyst samples for the FTS reaction was measured in a continuous stirred tank slurry reactor under the reaction conditions ofn(H2)/n(CO)=0.67, WHSV=2000h-1, 1.5 MPa, and 250 ℃. The results showed that the addition of SO2-4 promoted the reduction of the catalyst in H2. A low level of SO2-4 slightly influenced the extent of carburization, and the excessive addition of SO2-4 restrained carburization apparently in syngas. The catalyst samples with different SO2-4 amounts displayed different FTS reactivity, but all the samples were stable during 500 h on stream. Moreover, the addition of SO2-4 could suppress the water-gas shift reaction. The low level of SO2-4 suppressed methane selectivity and promoted slightly alkene selectivity.

Key words: sulfate, Fischer-Tropsch synthesis, iron-based catalyst, slurry reactor