物理化学学报 >> 2015, Vol. 31 >> Issue (7): 1391-1398.doi: 10.3866/PKU.WHXB201504303

催化和表面科学 上一篇    下一篇

Sn改性的Ru/H-CMK-3催化剂的制备及其肉桂醛选择性加氢性能的研究

高爽, 颜见标, 丛德全, 随强盛, 夏延洋, 程东东, 包强, 王振旅, 王力彦   

  1. 吉林大学化学学院, 吉林省表面与界面化学重点实验室, 长春130021
  • 收稿日期:2015-02-12 修回日期:2015-04-30 发布日期:2015-07-08
  • 通讯作者: 王振旅, 王力彦 E-mail:wzl@jlu.edu.cn;wangliyan@vip.sina.com
  • 基金资助:

    国家自然科学基金(21473074),吉林省科技攻关计划重点科技攻关项目(20150204020GX)和吉林省科技厅自然科学基金项目(20130101015JC)资助

Preparation of Sn-Modified Ru/H-CMK-3 Catalysts and Their Application in the Hydrogenation of Cinnamaldehyde

GAO Shuang, YAN Jian-Biao, CONG De-Quan, SUI Qiang-Sheng, XIA Yan-Yang, CHENG Dong-Dong, BAO Qiang, WANG Zhen-Lü, WANG Li-Yan   

  1. Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, P. R. China
  • Received:2015-02-12 Revised:2015-04-30 Published:2015-07-08
  • Contact: WANG Zhen-Lü, WANG Li-Yan E-mail:wzl@jlu.edu.cn;wangliyan@vip.sina.com
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21473074), Key Scientific Research Project of Jilin Province Science and Technology Development Plans, China (20150204020GX), and Natural Science Foundation of Science and Technology Department of Jilin Province, China (20130101015JC).

摘要:

用浸渍-原位还原法制备了Ru-Sn/H-CMK-3催化剂. 以肉桂醛选择性加氢制备肉桂醇为探针反应. 详细研究了催化剂的制备及反应条件对肉桂醛选择性加氢性能的影响. 采用X 射线粉末衍射(XRD)、比表面积(BET)、X光电子能谱(XPS)、透射电镜(TEM)等手段对催化剂结构和性质进行了表征. 结果表明, 介孔CMK-3碳材料能够更好地分散活性物种. 添加适量的Sn(IV)有利于Ru处于电子富集状态. 催化剂的主要活性物种是纳米Ru粒子, Ru和Sn之间的相互作用更加有利于C=O的活化. 同时, 反应温度和反应压力等条件的变化对肉桂醛选择性加氢制备肉桂醇反应也具有较大的影响.

关键词: 钌, 介孔碳, 肉桂醛, 肉桂醇, 催化加氢

Abstract:

Tin-promoted Ru/H-CMK-3 catalysts were prepared by a novel reductant-impregnation method for application in the hydrogenation of cinnamaldehyde. The catalysts were characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) specific surface areas, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The effects of the synthesis reaction conditions on the selective hydrogenation of cinnamaldehyde were examined in detail. The results showed that the mesoporous CMK-3 carbon material could disperse the catalytically active species better. Using appropriate amounts of Sn(IV) provided electron-rich Ru sites, which are one of the main catalytically active species. The interaction between Ru and Sn promoted the activation of C=O in cinnamaldehyde. Furthermore, changes in other reaction conditions, such as temperature and pressure, greatly influenced the selective hydrogenation of cinnamaldehyde.

Key words: Ruthenium, Mesoporous carbon, Cinnamaldehyde, Cinnamyl alcohol, Catalytic hydrogenation

MSC2000: 

  • O643