催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (12): 1452-1456.DOI: 10.3724/SP.J.1088.2010.00539

• 研究论文 • 上一篇    下一篇

Ru 前驱体对 Ru/MgO-CeO2 氨合成催化剂性能的影响

王秀云, 王榕, 倪军, 林建新, 魏可镁   

  1. 福州大学化肥催化剂国家工程研究中心, 福建福州 350002
  • 收稿日期:2010-05-27 出版日期:2010-12-13 发布日期:2014-04-26

Effect of Precursors on Catalytic Activity of Ru/MgO-CeO2 Catalyst for Ammonia Synthesis

WANG Xiuyun, WANG Rong*, NI Jun, LIN Jianxin, WEI Kemei   

  1. National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
  • Received:2010-05-27 Online:2010-12-13 Published:2014-04-26

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摘要： 分别以 K2RuO4, Ru(Ac)3 和 RuCl3 为 Ru 前驱体, 制备了 Ru/MgO-CeO2 催化剂, 并运用 X 射线衍射、X 射线荧光光谱, CO 吸附、N2 物理吸附和 H2程序升温还原等技术对催化剂进行了表征, 考察了 Ru 前驱体对 Ru/MgO-CeO2 催化剂氨合成性能的影响. 结果表明, Ru 前驱体对载体 MgO-CeO2 和 Ru 的还原性能、氯残留量和催化剂比表面积的影响都很大, 从而导致催化剂的氨合成性能的不同. 其中以 K2RuO4 为 Ru 前驱体制备的催化剂的载体和 Ru 容易还原, 无氯离子, 且比表面积较高, 因而催化剂活性和氨合成转换频率较高. 在 10 MPa, 425 °C, 10 000 h-1 条件下, K2RuO4, Ru(Ac)3 和 RuCl3 作前驱体制备的催化剂上氨合成转换频率比为 1.33:1.05:1.

关键词: 前驱体, 氨合成, 氧化镁, 二氧化铈, 钌

Abstract: Ru/MgO-CeO2 catalysts were prepared by co-precipitation with different precursors, including K2RuO4, Ru(Ac)3, and RuCl3, the obtained catalysts were characterized by X-ray diffraction, X-ray fluorescence, N2 physisorption, temperature-programmed reduction, and CO chemisorption. The results showed that the ammonia synthesis activity of the Ru/MgO-CeO2 catalyst prepared with K2RuO4 was 16.0% at 10 MPa, 450 °C, and 10 000 h-1, which was higher than those obtained with the other two precursors. The turnover frequency (TOF) of the Ru/MgO-CeO2 catalyst prepared with K2RuO4 was higher than those obtained with the other precursors under the same reaction conditions. The influence of precursors and preparation methods on the structure and performance of the catalysts was studied. The ratio of Ru/MgO-CeO2 catalysts prepared with K2RuO4, Ru(Ac)3, and RuCl3 as precursors for ammonia synthesis turnover frequency is 1.33:1.05:1 under 10 MPa, 425 °C, and 10 000 h-1.

Key words: precursor, ammonia synthesis, magnesium oxide, cerium dioxide, ruthenium