催化学报 ›› 2006, Vol. 27 ›› Issue (8): 659-663.

• 研究论文 • 上一篇    下一篇

Ni/La2O3/α-Al2O3中的高温脱附氢促进CH4/CO2重整反应的初活性

崔月华,徐恒泳,葛庆杰,毕亚东,王玉忠,侯守福,李文钊   

  1. 中国科学院大连化学物理研究所, 辽宁大连 116023
  • 收稿日期:2006-08-25 出版日期:2006-08-25 发布日期:2010-09-28

High Temperature Desorbed Hydrogen in Ni/La2O3/α-Al2O3 Improves the Initial Reaction Rate of CH4/CO2 Reforming

CUI Yuehua, XU Hengyong*, GE Qingjie, BI Yadong, WANG Yuzhong, HOU Shoufu, LI Wenzhao   

  1. Dalian Institute of Chemical Physics, The Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • Received:2006-08-25 Online:2006-08-25 Published:2010-09-28

摘要: 通过H2程序升温脱附实验,在H2还原的Ni/La2O3/α-Al2O3催化剂上可以明显观察到高温脱附氢(高温氢). 动力学实验结果表明,随催化剂上高温氢含量的增加, CH4/CO2重整反应的初始活性升高,同时高温氢也可在重整反应过程中原位生成,并使重整反应的活性最终达到稳定. 脉冲实验结果表明,随催化剂上高温氢含量的增加, CH4解离后生成的活性中间体CHx物种的x值也增大,进而降低了CHx与CO2反应的活化能,提高了CHx与CO2反应的速率. La2O3助剂的添加提高了Ni/La2O3/α-Al2O3催化剂上逆水气变换反应的速率,并且对CO2的活化也有促进作用. La2O3助剂的加入对于CH4/CO2重整反应的重要作用是使高温氢的数量增多且稳定性提高,有利于保持CHx物种中较高的x值,促进重整反应.

关键词: 高温脱附氢, 镍基催化剂, 氧化镧, 甲烷重整反应, 初始速率

Abstract: The hydrogen desorbed at high temperature (high-temperature hydrogen) over the hydrogen reduced catalyst Ni/La2O3/α-Al2O3 was observed by H2 temperature-programmed desorption. Kinetic experiments show that the activity of the reforming reaction is initially increased with the amount of high-temperature hydrogen in Ni/La2O3/α-Al2O3 and finally reaches a constant value due to the in situ generation of the high-temperature hydrogen. Pulse results indicate that the high-temperature hydrogen in Ni/La2O3/α-Al2O3 is prone to form CHx species with high x values, which has higher activity for the reaction of CHx with CO2. The Ni/La2O3/α-Al2O3 catalyst with plenty of high-temperature hydrogen can increase the x values of CHx species and decrease the activation energy for the reaction between CHx and CO2, leading to a higher reaction rate. The addition of La2O3 on the Ni/α-Al2O3 catalyst promotes the reverse water-gas shift reaction and slightly improves the activation of CO2. La2O3 also increases the amount of high-temperature hydrogen and its stability, resulting in higher x values of CHx species and improving the reforming reaction rate.

Key words: high-temperature desorbed hydrogen, nickel-based catalyst, lanthana, methane reforming reaction, initial rate