化学学报 ›› 2004, Vol. 62 ›› Issue (18): 1717-1720. 上一篇    下一篇

研究论文

F离子对钌基氨合成催化剂活性的影响

林敬东1, 黄桂玉2, 许宗祥1, 廖代伟1,3,4   

  1. 1. 厦门大学化学系, 厦门, 361005;
    2. 厦门大学化学工程与生物工程系, 厦门, 361005;
    3. 厦门大学固体表面物理化学国家重点实验室, 厦门, 361005;
    4. 厦门大学物理化学研究所, 厦门, 361005
  • 投稿日期:2004-04-07 修回日期:2004-06-10 发布日期:2014-02-17
  • 通讯作者: 廖代伟,E-mail:dwliao@xmu.edu.cn E-mail:dwliao@xmu.edu.cn
  • 基金资助:
    国家自然科学基金(Nos.20273053,20023001,29933040)和国家重点基础研究发展规划(No.001CB108906)资助项目.

Effects of Fluoride on Activities of Ru-based Ammonia Synthesis Catalysts

LIN Jing-Dong1, HUANG Gui-Yu2, XU Zong-Xiang1, LIAO Dai-Wei1,3,4   

  1. 1. Department of Chemistry, Xiamen University, Xiamen 361005;
    2. Department of Chemical and Biochemical Engineering, Xiamen University, Xiamen 361005;
    3. State Key Laboratory for Physical Chemistry of Solid Surface, Xiamen University, Xiamen 361005;
    4. Institute of Physical Chemistry, Xiamen University, Xiamen 361005
  • Received:2004-04-07 Revised:2004-06-10 Published:2014-02-17

以MgO为载体,分别用KF,KNO3,BaF2和BaO为促进剂前驱体制备钌基氨合成催化剂,并用X射线衍射(XRD)、高分辨透射电子显微镜(HRTEM)和催化剂性能评价等方法考察了不同促进剂前驱体对钌基氨合成催化剂的影响.结果表明,电负性比氯大的氟的引入能提高催化剂的活性,在KF-Ru/MgO催化剂中,F与载体的O发生交换,改变了载体的结构和表面性质,从而导致金属载体相互作用情况的不同以及金属分散度的提高,因而有利于催化活性的提高.同时,当F以BaF2的形态存在时也能提高催化活性.

关键词: 氨合成, 钌, 氟化物, 促进剂

A series of Ru based ammonia synthesis catalysts supported by magnesia with different promoter precursors were prepared. The effects of different promoter precursors on the catalysts were investigated by XRD, HRTEM and performance evaluation techniques. The results indicated that the activities of catalysts were increased by the introduction of fluoride and some oxygen of magnesia was exchanged with fluoride in KF-Ru/MgO catalyst. It was suggested that the exchange of oxygen and fluoride changed the structure and surface property of support, hence improving the metal dispersion and the different interactions of ruthenium and the support. Consequently, the activity of catalyst prepared with KF was higher. At the same time, the activity of catalyst prepared by BaF2 was also higher than the one prepared by BaO, though the configuration of fluoride and barium was BaF2.

Key words: ammonia synthesis, ruthenium, fluoride, promoter