催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (9): 1162-1166.DOI: 10.3724/SP.J.1088.2010.00148

• 研究论文 • 上一篇    下一篇

阶跃升温分解法对非负载型镍催化甲烷分解活性的影响

张微1,2, 葛庆杰1, 徐恒泳1   

  1. 1 中国科学院大连化学物理研究所, 辽宁大连 116023 2 中国科学院研究生院, 北京 100049
  • 收稿日期:2010-09-30 出版日期:2010-09-30 发布日期:2014-01-25

Influence of Step Temperature Elevating Decomposition on the Catalytic Activity of Non-supported Ni for Methane Decomposition

ZHANG Wei1,2, GE Qingjie1,*, XU Hengyong1,*   

  1. 1Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2010-09-30 Online:2010-09-30 Published:2014-01-25

PDF

707

被引次数

8

摘要： 以乙醇为洗涤溶剂采用沉淀法制备了非负载型 Ni 催化剂, 考察了预处理过程对催化剂上 CH4 分解活性的影响. X 射线衍射及 CH4 程序升温表面反应结果表明, 降低还原温度可减小 Ni 粒子尺寸, 从而提高催化剂活性. 同时, 采用 CH4 多温度逐步分解 (多点阶跃升温分解) 法可形成较稳定的 Ni 粒子, 有效提高催化剂的活性及稳定性, 500 oC 下 CH4 初始转化率可达 8.40%, 反应 120 min 时升至 11.20%; 而在 350 和 500 oC 两点阶跃升温分解的 CH4 最高转化率只有 1.61%.

关键词: 甲烷, 阶跃升温分解, 非负载型镍催化剂, 分解活性

Abstract: The non-supported Ni catalyst was prepared by calcination of the nickel hydroxide precipitate, originated from precipitation of nickel acetate with aqueous solution of sodium carbonate, rinsed with ethanol. The influence of pretreatment conditions on Ni catalyst was investigated by means of X-ray diffraction, CH4 temperature-programmed surface reaction, and CH4 decomposition reactivity test. The results showed that lowering the reduction temperature could reduce Ni particle size and correspondingly improve the catalytic activity of Ni catalyst for CH4 decomposition. The result of the catalytic activity test showed that reaction history was an important factor influencing the catalytic activity of the Ni catalyst for CH4 decomposition at 500 oC. The formation of relatively stable Ni particles could be realized by carrying out CH4 decomposition stepwise at multiple reaction temperatures (multiple step temperature elevating decomposition), which could remarkably improve the catalytic activity and stability of the Ni catalyst for CH4 decomposition. The initial CH4 conversion reached 8.40% at 500 oC by using the multiple step temperature elevating decomposition method, and the CH4 conversion could further be increased to 11.20% within 120 min, whereas by the two step temperature elevating decomposition method, the maximum CH4 conversion at 500 oC was only 1.61%.

Key words: methane, step temperature elevating decomposition, non-supported nickel catalyst, decomposition reactivity