应用化学 ›› 2011, Vol. 28 ›› Issue (08): 936-941.DOI: 10.3724/SP.J.1095.2011.00552

• 研究论文 • 上一篇    下一篇

超临界甲醇处理对活性炭表面性质及钌炭催化性能的影响

徐三魁1,2,王晓栋1,李利民1*,许群3,李蕊1   

  1. (1.郑州大学化学系 郑州 450052;2.河南工业大学材料科学与工程学院 郑州;
    3.郑州大学材料科学与工程学院 郑州 )
  • 收稿日期:2010-09-20 修回日期:2010-12-06 出版日期:2011-08-10 发布日期:2011-08-10
  • 通讯作者: 李利民,教授; Tel:0371-67763046; Fax:0371-67758729; E-mail:lilm@zzu.edu.cn; 研究方向:催化新技术、催化新材料
  • 基金资助:
    河南省教育厅基金资助项目(2010A150008)

Effect of Supercritical Methanol Treatment on the Surface Property of Activated Carbon and the Activity of Ru/Activated Carbon Catalyst

XU Sankui1,2, WANG Xiaodong1, LI Limin1*, XU Qun3, LI Rui1   

  1. (1.Department  of  Chemistry,Zhengzhou University,Zhengzhou 450052;
    2.College of Material Engineering,Henan University of Technology,Zhengzhou;
    3.College of Material Engineering,Zhengzhou University,Zhengzhou)
  • Received:2010-09-20 Revised:2010-12-06 Published:2011-08-10 Online:2011-08-10

摘要:

采用超临界甲醇处理活性炭,水浸渍制备负载钌炭催化剂,用N2物理吸附、Boehm滴定、X光电子能谱(XPS)和程序升温还原(TPR)等测试技术研究了超临界甲醇处理对活性炭表面结构及表面基团相对含量的影响,并以葡萄糖加氢生产山梨醇为模型反应对钌基催化剂的性能进行了评价。 研究结果表明,超临界甲醇处理活性炭,活性炭的孔结构性能变化不大,但可有效降低活性炭表面含氧酸性基团的含量,使催化剂的还原温度升高,增强了载体和活性组分间的相互作用,有效的提高了钌的分散度,从而提高所负载催化剂的催化活性。 在实验范围内,当超临界甲醇的温度为300 ℃,处理时间为12 h时,在4.0 MPa、120 ℃、葡萄糖的质量分数为50%的反应条件下,催化剂的反应速率(按Ru单位质量计)达到了118.65 mmol/(min·g),是未处理活性炭的1.96倍。

关键词: 超临界, 钌基催化剂, 表面基团, 葡糖糖加氢, 活性炭

Abstract:

Activated carbon(AC) was modified by supercritical fluidic methanol in order to obtain materials with different surface properties. Several techniques were used to characterize the activated carbon and Ru/AC catalysts including N2 physisorption, Boehm titration, XPS and temperature-programmed reduction(TPR). The results show that supercritical fluid treatment does not remarkably change the surface structure of activated carbon, but significantly reduce the amount of the surface acidic groups. Thus Ru deposited on them will assemble. These led to a higher dispersion of Ru and enhanced the activity of the catalysts prepared by impregnation of AC supported with RuCl3 solution. The activities of Ru/AC catalysts for hydrogenation of glucose were tested under 4.0 MPa and 120 ℃. The results show that activities of Ru/AC catalysts prepared by supercritical fluid treatment are increased, and the highest reaction rate(in Ru mass unit) for hydrogenation of glucose reaches 118.65 mmol/(min·g), which was 1.96 times higher than that without treatment.

Key words: supercritical fluid, ruthenium catalyst, surface group, glucose hydrogenation, activated carbon

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