物理化学学报 >> 2015, Vol. 31 >> Issue (4): 729-737.doi: 10.3866/PKU.WHXB201501292

催化和表面科学 上一篇    下一篇

具有特殊结构和电子性质的PdAu/Al2O3催化剂上蒽醌加氢反应性能

韩优, 何志远, 管永川, 李韡, 张金利   

  1. 天津大学化工学院, 天津300072
  • 收稿日期:2014-11-26 修回日期:2015-01-28 发布日期:2015-04-03
  • 通讯作者: 张金利 E-mail:zhangjinli@tju.edu.cn
  • 基金资助:

    国家自然科学基金委(21106094, 21276179), 国家重点基础研究规划项目(2012CB720300)和长江学者与创新团队发展计划(IRT1161)资助

Catalytic Performance of PdAu/Al2O3 Catalyst with Special Structural and Electronic Properties in the 2-Ethylanthraquinone Hydrogenation Reaction

HAN You, HE Zhi-Yuan, GUAN Yong-Chuan, LI Wei, ZHANG Jin-Li   

  1. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China
  • Received:2014-11-26 Revised:2015-01-28 Published:2015-04-03
  • Contact: ZHANG Jin-Li E-mail:zhangjinli@tju.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21106094, 21276179), National Key Basic Research Program of China (973) (2012CB720300), and Program for Changjiang Scholars, Innovative Research Team in University, China (IRT1161).

摘要:

通过改变Pd和Au的负载顺序合成了一系列具有不同结构和电子性质的PdAu双金属催化剂, 并用于蒽醌加氢反应. 其中通过先负载Au后负载Pd的顺序制得的Pd/Au/Al2O3催化剂, 其加氢效率可高达14.27 g·L-1.X射线衍射、透射电子显微镜、H2程序升温还原和X射线光电子能谱等分析表征结果显示, Pd/Au/Al2O3催化剂中分散在Au颗粒表面的Pd纳米颗粒具有独特的爆米花结构, 其表面零价态的单质Pd含量最多, 而这种表面零价态的单质Pd是蒽醌加氢反应中的关键活性组分. 此外, Au的加入可有效抑制副反应的发生, 减少降解产物的生成, 从而大大提高了催化选择性.

关键词: 负载顺序, PdAu双金属, 蒽醌加氢, 降解产物

Abstract:

A series of bimetallic PdAu catalysts with different structures were prepared by changing the loading sequence of Pd and Au for the hydrogenation of 2-ethylanthraquinone. Pd/Au/Al2O3 was obtained by loading Pd onto Au particles deposited onto an Al2O3 support with a hydrogenation efficiency up to 14.27 g·L-1. According to X-ray diffraction, transmission electron microscopy, hydrogen temperature program reduction, and X-ray photoelectron spectroscopy measurements, the popcorn structure and unique electronic properties of the Pd species in the Pd/Au/Al2O3 catalyst resulted in the highest content of surface metallic Pd, which was the most active component for the reaction. What is more, the addition of Au can effectively reduce the amount of degradation products by suppressing side reactions.

Key words: Loading sequence, Bimetallic PdAu, Anthraquinone hydrogenation, Degradation product

MSC2000: 

  • O643