物理化学学报 >> 2010, Vol. 26 >> Issue (10): 2719-2725.doi: 10.3866/PKU.WHXB20101022

催化和表面结构 上一篇    下一篇

负载型非晶态Co-B催化剂在1-辛烯氢甲酰化中的应用

龙俊英1, 马兰1,2, 贺德华1   

  1. 1. 清华大学化学系, 有机光电子与分子工程教育部重点实验室,分子催化与定向转化研究室,北京 100084;
    2. 防化指挥工程学院, 北京 102205
  • 收稿日期:2010-04-26 修回日期:2010-06-24 发布日期:2010-09-27
  • 通讯作者: 贺德华 E-mail:hedeh@mail.tsinghua.edu.cn
  • 基金资助:

    国家自然科学基金(20921001)资助项目

1-Octene Hydroformylation Using Supported Amorphous Co-B Catalysts

LONG Jun-Ying1, MA Lan1,2, HE De-Hua1   

  1. 1. Innovative Catalysis Program, Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China;
    2. Institute of Chemical Defence, Beijing 102205, P. R. China
  • Received:2010-04-26 Revised:2010-06-24 Published:2010-09-27
  • Contact: HE De-Hua E-mail:hedeh@mail.tsinghua.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20921001).

摘要:

以醇凝胶-氮气热处理方法制备的ZrO2、碳纳米管(CNTs) 及介孔分子筛SBA -15作为载体, 采用化学还原法制备了负载型非晶态Co-B催化剂, 利用粉末X 射线衍射(XRD) 、氮气吸附等温线、透射电子显微镜(TEM) 、电感耦合等离子体-原子发射光谱(ICP-AES) 以及X 射线光电子能谱(XPS) 等对催化剂进行了表征. 以1-辛烯的氢甲酰化为目标反应, 考察了负载型非晶态Co-B 催化剂在氢甲酰化反应中的性能及循环使用效果. 表征结果显示, 以NaBH4 为还原剂制备的负载型Co-B 催化剂上的Co-B 为非晶态, 负载Co-B 组分对载体的晶相结构没有影响. 反应结果表明, 在1-辛烯的氢甲酰化反应中, 负载型非晶态Co-B 催化剂都显示较高的初始活性. 随着循环次数的增加, 三种催化剂的活性下降, 但下降幅度有所不同, Co-B/CNTs 和Co-B/SBA-15 的循环使用稳定性高于Co-B/ZrO2.

关键词: Co-B 非晶态催化剂, 负载, 氢甲酰化, 催化性能

Abstract:

Co-B catalysts supported on ZrO2 (prepared by alcogel nitrogen thermo-treatment method), carbon nanotubes (CNTs), and mesoporous SBA-15 as supports were prepared by chemical reduction method and characterized by X-ray diffraction (XRD), nitrogen physisorption, transmission electron microscopy (TEM), inductively coupled plasma -atomic emission spectrometry (ICP-AES) and X-ray photoelectron spectroscopy (XPS). Hydroformylation of 1-octene was used as a probe reaction to investigate the catalytic performance and stability of the catalysts in recycles. The as-prepared Co-B catalysts showed amorphous characteristics and the support structures were unchanged. The reaction results reveal that the catalytic activities of Co-B/CNTs, Co-B/ZrO2 and Co-B/SBA-15 in the hydroformylation of 1-octene were comparatively high. However, the catalytic activities decreased upon recycling. Nevertheless, the Co-B/ CNTs and Co-B/SBA-15 were relatively stable compared with Co-B/ZrO2.

Key words: Amorphous Co-B catalyst, Support, Hydroformylation, Catalytic property

MSC2000: 

  • O643