物理化学学报 >> 2012, Vol. 28 >> Issue (03): 667-673.doi: 10.3866/PKU.WHXB201112221

催化和表面科学 上一篇    下一篇

单分散SiO2的焙烧温度对Rh基催化剂上CO加氢反应性能的影响

俞俊1,2, 毛东森2, 郭强胜2, 韩璐蓬2, 卢冠忠1,2   

  1. 1. 华东理工大学工业催化研究所, 上海 200237;
    2. 上海应用技术学院应用催化研究所, 上海 201418
  • 收稿日期:2011-10-11 修回日期:2011-12-01 发布日期:2012-02-23
  • 通讯作者: 毛东森, 卢冠忠 E-mail:dsmao@sit.edu.cn; gzhlu@ecust.edu.cn
  • 基金资助:

    上海市科委(08520513600), 上海市教委重点学科建设(J51503)和上海市优秀青年教师专项基金(yyy10083)资助项目

Effect of Calcination Temperature of Monodispersed SiO2 on the Performance of Rh-Based Catalysts for CO Hydrogenation

YU Jun1,2, MAO Dong-Sen2, GUO Qiang-Sheng2, HAN Lu-Peng2, LU Guan-Zhong1,2   

  1. 1. Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, P. R. China;
    2. Research Institute of Applied Catalysis, Shanghai Institute of Technology, Shanghai 201418, P. R. China
  • Received:2011-10-11 Revised:2011-12-01 Published:2012-02-23
  • Contact: MAO Dong-Sen, LU Guan-Zhong E-mail:dsmao@sit.edu.cn; gzhlu@ecust.edu.cn
  • Supported by:

    The project was supported by the Science and Technology Commission of Shanghai Municipality, China (08520513600), Leading Academic Discipline Project of Shanghai Education Committee, China (J51503), and Shanghai Special Fund for Outstanding Young Teachers, China (yyy10083).

摘要: 在比较了分别以商业SiO2和采用Stöber 法制备的单分散SiO2为载体的Rh-Mn-Li/SiO2催化剂催化CO加氢反应性能的基础上, 进一步调变了Stöber 法制备SiO2时的焙烧温度, 并考察了其对Rh-Mn-Li/SiO2催化CO加氢性能的影响. 利用N2吸附-脱附、傅里叶变换红外(FTIR)光谱、H2程序升温还原(H2-TPR)、程序升温表面反应(TPSR)等方法对载体及催化剂的物理化学性能进行了表征. 结果表明: 不同温度焙烧的载体表面具有不同的Si―OH数量, 从而影响金属的分散状态及Rh和Mn之间的相互作用. 载体表面较多的羟基有利于Rh的分散和CO的吸附, 从而增强催化剂的反应活性. 载体表面适当数量的羟基能够得到适中的Rh与Mn之间的相互作用, 使催化剂具有合适的CO解离能力, 有利于CHx的CO插入反应, 从而提高了C2含氧化合物的选择性.

关键词: Rh-Mn-Li/SiO2, CO加氢, C2含氧化合物, 焙烧温度

Abstract: Based on a comparison of catalytic performances of Rh-Mn-Li/SiO2 catalysts, in which commercial SiO2 and monodispersed SiO2 synthesized by the Stöber method were used as the support, respectively, the effect of the calcination temperature of the synthesized SiO2 on the catalytic performance of Rh-Mn-Li/SiO2 for CO hydrogenation to C2 oxygenates was investigated. Fourier transform infrared spectroscopy, N2 adsorption-desorption, temperature-programmed reduction with hydrogen (H2-TPR), and temperature-programmed surface reaction (TPSR) were used to characterize the physico-chemical properties of the SiO2 supports and the corresponding catalysts. The results showed that the number of surface Si―OH groups on the SiO2 supports affected the dispersion of metal and the interaction between Rh and Mn. Large amount of surface Si―OH groups was favorable for the dispersion of Rh particles and CO adsorption, and enhanced the activity of the catalyst. An appropriate amount of Si ―OH groups can gain moderate interaction between the Rh and Mn. This interaction is conducive to achieve the right CO dissociation ability, which is favorable for the insertion of CO to CHx, and ultimately increases the selectivity of C2 oxygenates.

Key words: Rh-Mn-Li/SiO2, CO hydrogenation, C2 oxygenate, Calcination temperature

MSC2000: 

  • O643