催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (7): 1075-1079.DOI: 10.1016/S1872-2067(11)60413-0

• 研究快讯 • 上一篇    下一篇

柠檬酸络合法制备 Ba 促进 ZrO2 负载 Ru 催化剂上氨合成反应性能

林建新*, 王自庆, 张留明, 倪军, 王榕, 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:2012-04-23 修回日期:2012-05-20 出版日期:2012-06-21 发布日期:2012-06-21

Ammonia Synthesis over Ruthenium Catalysts using Barium-Doped Zirconia as Supports Prepared by Citric Acid Method

LIN Jianxin*, WANG Ziqing, ZHANG Liuming, NI Jun, WANG Rong, WEI Kemei   

  1. National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
  • Received:2012-04-23 Revised:2012-05-20 Online:2012-06-21 Published:2012-06-21

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摘要： 采用柠檬酸络合法制备了一系列不同含量 Ba 掺杂的 ZrO2, 再用浸渍法制备了 K-Ru/Ba-ZrO2 催化剂并将其用于氨合成反应. 采用 X 射线衍射和 CO2 程序升温脱附技术考察了 Ba 含量对催化剂结构与性能的影响. 结果表明, Ba 掺入 ZrO2 后形成的 BaZrO3 有助于其负载的 Ru 催化剂氨合成活性的显著提高. 在 5.0 MPa, 10000 h-1, 425 oC 时, Ru/Ba-ZrO2 (Ba:Zr 摩尔比为 1:1) 催化剂活性最高, 出口氨浓度和反应速率分别达 9.24% 和 29.77 mmol/(g•h). 这主要归因于载体的强电子传导性能和碱性提高.

关键词: 钡, 二氧化锆, 钌, 氨合成, 电子作用

Abstract: Barium-promoted zirconia (Ba-ZrO2) was synthesized by the citric acid method and used as supports for Ru/Ba-ZrO2 catalysts, which were prepared by incipient wetness impregnation with K2RuO4 as precursor. The obtained Ba-ZrO2 and catalysts were characterized by X-ray diffraction and CO2 temperature-programmed desorption. The effect of Ba content on the structure and catalytic activity of K-Ru/Ba-ZrO2 catalysts is discussed. The formation of BaZrO3 can improve significantly the catalytic activity of Ru/Ba-ZrO2 for ammonia synthesis. The ammonia concentration and rate of ammonia synthesis of the K-Ru/Ba-ZrO2 catalyst (molar ratio of Ba:Zr is 1:1) were 9.24% and 29.77 mmol/(g•h), respectively, at 425 °C, 5.0 MPa, and 10000 h-1. Improvements in electron conductivity and the basic nature of the catalyst may be the main reasons for such high catalytic activity in ammonia synthesis.

Key words: barium, zircona, ruthenium, ammonia synthesis, electronic conductivity