催化学报 ›› 2009, Vol. 30 ›› Issue (3): 218-222.

• 研究论文 • 上一篇    下一篇

稀土掺杂对纳米钡-氧化镁载体及其负载钌基氨合成催化剂性能的影响

霍超, 夏庆华, 杨霞珍, 骆燕, 刘化章   

  1. 浙江工业大学化学工程与材料学院, 浙江杭州310032
  • 收稿日期:2009-03-25 出版日期:2009-03-25 发布日期:2012-12-19

Effects of Rare Earth Doping on the Performance of Nano-Ba-Magnesia Supports and Ru-Based Catalysts for Ammonia Synthesis

HUO Chao*, XIA Qinghua, YANG Xiazhen, LUO Yan, LIU Huazhang   

  1. College of Chemical Engineering and Materials Science, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China
  • Received:2009-03-25 Online:2009-03-25 Published:2012-12-19

摘要: 利用超声-共沉淀技术制备了一系列稀土与钡共掺杂的纳米氧化镁载体(RE-Ba-MgO, RE = La, Sm和Ce)及其负载的钌基氨合成催化剂(Ru/RE-Ba-MgO). 通过氮气物理吸附、X射线衍射、场发射扫描电镜、热重分析仪及H2程序升温还原等方法对载体和催化剂进行了表征. 结果表明, Ba在载体中的掺杂形式分为低温分解型BaCO3和高温分解型BaCO3. 稀土的掺杂可明显改变载体的表面形态及表面结构, 使载体化学与结构性能发生变化, 从而导致低温分解型BaCO3的相对含量发生变化, 进而改变催化剂的低温活性. 在10 MPa, 400 oC, 10 000 h?1的测试条件下, Ru/La-Ba-MgO催化剂的出口氨浓度达到65.49 mmol/(g•h), 比Ru/Ba-MgO催化剂活性提高了66.3%.

关键词: 稀土, 掺钡纳米氧化镁, 钌基催化剂, 氨合成, 超声制备

Abstract: The Ru catalysts were prepared by the impregnation method using rare earth (La, Sm, and Ce) and barium-doped nano- magnesia (RE-Ba-MgO) as the supports. The Ru/La-Ba-MgO catalyst showed the highest catalytic activity for the ammonia synthesis with a reaction rate of 65.49 mmol/(g•h) at 10 MPa, 400 oC, and 10 000 h?1, upgrading 66.3% compared with Ru/Ba-MgO. It would be valuable for the development of effective and applicable catalysts for the ammonia synthesis industry.

Key words: rare earth, barium-doped nano-magnesia, ruthenium catalyst, ammonia synthesis, ultrasonic preparation