物理化学学报 >> 2008, Vol. 24 >> Issue (06): 965-970.doi: 10.3866/PKU.WHXB200806081

研究论文 上一篇    下一篇

Ru/ZrO2·xH2O催化喹啉加氢反应

张瑞敏; 樊光银; 李诚; 王瑛瑛; 李瑞祥; 陈华; 李贤均   

  1. 四川大学化学学院有机金属络合催化研究所, 绿色化学与技术教育部重点实验室, 成都 610064
  • 收稿日期:2008-01-08 修回日期:2008-02-22 发布日期:2008-06-03
  • 通讯作者: 陈华 E-mail:scuhchen@163.com

Hydrogenation of Quinoline over Ru/ZrO2·xH2O

ZHANG Rui-Min; FAN Guang-Yin; LI Cheng; WANG Ying-Ying; LI Rui-Xiang; CHEN Hua; LI Xian-Jun   

  1. Key Laboratory of Green Chemistry and Technology of the Ministry of Education, Institute of Homogeneous Catalysis, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China
  • Received:2008-01-08 Revised:2008-02-22 Published:2008-06-03
  • Contact: CHEN Hua E-mail:scuhchen@163.com

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摘要： 制备了负载型催化剂Ru/ZrO2·xH2O, 并用XRD、XPS和TEM对催化剂进行了表征, 所制得的催化剂金属钌的平均粒径约为3.8 nm. 在2 MPa和40 ℃的温和条件下, 以水为溶剂时, Ru/ZrO2·xH2O催化喹啉加氢生成1,2,3,4-四氢喹啉的选择性达98.0%, 而且表现出较强的抗氮中毒能力, 催化剂循环使用性能稳定. 对喹啉加氢反应中的催化反应机理进行了探讨.

关键词: 钌, 二氧化锆, 负载型催化剂, 喹啉, 加氢, 四氢喹啉

Abstract: The highly dispersed supported catalyst (Ru/ZrO2·xH2O) was prepared and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microsocpy. The results showed that ruthenium was reduced to low oxidation state and the average partical diameter of Ru particles was about 3.8 nm. The catalyst exhibited high activity in hydrogenation of quinoline under the mild reaction conditions, 40 ℃, 2 MPa, quinoline/Ru molar ratio of 250/1 and H2O as solvent. The conversion of quinoline was 98.2% and the selectity of 1,2,3,4-tetrahydroquinoline was 98.0%. The catalyst can be reused for several times. The mechanismof quinoline hydrogenation over Ru/ZrO2·xH2Ocatalyst was discussed. The coordination of nitrogen atomof quinoline on the surface of ruthenium nanoparticles and the effect of hydrogen bond between OH groups on ZrO2 surface and nitrogen in quinoline were favourable for the desorption of the substrate and products fromthe surface of catalyst.

Key words: Ruthenium, Zirconia, Supported catalyst, Quinoline, Hydrogenation, Tetrahydroquinoline

MSC2000: 

  • O643