催化学报 ›› 2013, Vol. 34 ›› Issue (4): 651-658.DOI: 10.1016/S1872-2067(12)60535-X

• 研究快讯 • 上一篇    下一篇

Ni基催化剂上木质素模型化合物苯基苯乙醚C-O键的加氢裂解

宋奇a,b, 蔡嘉莹a,b, 张俊杰a,b, 于维强a, 王峰a, 徐杰a   

  1. a 中国科学院大连化学物理研究所, 辽宁大连116023;
    b 中国科学院大学, 北京100049
  • 收稿日期:2012-12-30 修回日期:2013-01-30 出版日期:2013-04-23 发布日期:2013-04-24
  • 通讯作者: 王峰,徐杰
  • 基金资助:

    国家自然科学基金(21073184, 21273231, 21233008); 中国科学院“百人计划”择优支持项目.

Hydrogenation and cleavage of the C-O bonds in the lignin model compound phenethyl phenyl ether over a nickel-based catalyst

SONG Qia,b, CAI Jiayinga,b, ZHANG Junjiea,b, YU Weiqianga, WANG Fenga, XU Jiea   

  1. a Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    b Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2012-12-30 Revised:2013-01-30 Online:2013-04-23 Published:2013-04-24
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21073184, 21273231, 21233008) and One Hundred Person Project of the Chinese Academy of Sciences.

摘要:

研究了Ni基催化剂上木质素模型化合物苯基苯乙醚中C-O-C键加氢裂解性能.结果表明,Ni/C催化剂显示出优异的加氢裂解能力,苯基苯乙醚的转化率达到99%以上.Ni/C催化剂的还原方法对裂解选择性有重要影响;氢气还原制备的Ni/C-H催化剂上,C-O-C键裂解选择性为85%.Ru/C和Pd/C催化剂上裂解选择性分别为40%和69%.采用碳热还原方法制备的Ni/C-C催化剂,可以实现高选择性加氢和裂解,C-O-C键裂解选择性达到99%以上,其中芳烃化合物收率为44%.这可能与镍组分和载体碳之间的相互作用有关.

关键词: 木质素模型化合物, 苯基苯乙醚, 加氢裂解, 镍基催化剂, 芳香化合物

Abstract:

Phenethyl phenyl ether (PPE) was selected as a typical lignin model compound and hydrogenated and cleaved over two readily accessible nickel-based catalysts, which could be easily separated from the product mixture. The results revealed that the reduction of the nickel catalyst with gaseous hydrogen produced a species capable of achieving higher activity towards C-O-C bond cleavage compared to the Ru/C and Pd/C catalysts. The selectivity of the C-O-C bond cleavage over the Ni/C catalyst was 85%, and higher than the corresponding values in the Ru/C (40%) and Pd/C (69%) systems. Using the carbothermal reduction method for the production of the Ni/C-C catalyst, the conversion and selectivity levels reached 99%, with 40% of the benzene rings in PPE being reserved. In comparison, no benzene ring containing products wer observed over the noble metal catalysts. This difference was attributed to the interaction between the carbon support and the nickel nanoparticles.

Key words: Lignin model compound, Phenethyl phenyl ether, Hydrogenation and cleavage, Nickel catalyst, Aromatic compound