催化学报 ›› 2012, Vol. 33 ›› Issue (12): 1883-1888.DOI: 10.1016/S1872-2067(11)60451-8

• 研究论文 • 上一篇    下一篇

高活性三维花型 Co-Ni/C 双金属催化剂用于邻氯硝基苯选择性加氢反应

解雅玲, 肖南, 凌铮, 柳月, 于畅, 邱介山*   

  1. 大连理工大学辽宁省能源材料化工重点实验室, 大连理工大学精细化工国家重点实验室, 辽宁大连 116024
  • 收稿日期:2012-07-20 修回日期:2012-08-16 出版日期:2013-01-18 发布日期:2012-12-18

Flower-Like Co-Ni/C Bimetallic Catalysts for the Selective Hydrogenation of o-Chloronitrobenzene

XIE Yaling, XIAO Nan, LING Zheng, LIU Yue, YU Chang, QIU Jieshan*   

  1. Carbon Research Laboratory, Liaoning Key Lab for Energy Materials and Chemical Engineering, State Key Lab of Fine Chemicals, Dalian University of Technology, Dalian 116024, Liaoning, China
  • Received:2012-07-20 Revised:2012-08-16 Online:2013-01-18 Published:2012-12-18

摘要: 采用简单的水热/溶剂热法, 经后续在氮气气氛中的热处理合成了三维花型 Co-Ni/C 双金属催化剂, 它由交织炭片构成, 金属纳米颗粒高度分散其中. 随着 Co/Ni 摩尔比的增加, 金属颗粒的粒径逐渐从 26 nm 减至 4 nm 左右. 将该催化剂用于邻氯硝基苯选择性加氢制备邻氯苯胺反应, 其催化活性最高为单金属催化活性的 2 倍. 这是由于 Co 和 Ni 物种之间存在协同效应. 氢气程序升温脱附结果显示, Co/Ni 合金的生成使得 Co50Ni50/C 催化剂产生了新的催化活性位, 因而其活性显著提高.

关键词: 钴, 镍, 纳米碳材料, 双金属催化剂, 协同效应, 邻氯硝基苯, 加氢反应

Abstract: Three dimensional flower-like Co-Ni/C bimetallic catalysts composed of interlaced carbon flakes with highly dispersed metal nanoparticles were synthesized by a facile hydrothermal/solvothermal process followed by a heat treatment in flowing N2. The sizes of the metal nanoparticles were from 26 to 4 nm, which became smaller as the Co/Ni molar ratio increased. The catalytic activities for the selective hydrogenation of o-chloronitrobenzene to o-chloroaniline were tested. The conversion of o-chloronitrobenzene over the bimetallic Co-Ni/C catalysts was increased by up to 200% compared with that over a mono-metallic Co/C catalyst, which was due to a synergistic interaction between the Co and Ni species. Hydrogen temperature-programmed desorption results showed that new active sites were formed in the Co50Ni50/C catalyst due to the formation of a Co-Ni alloy, which gave the improved activity of the Co50Ni50/C catalyst.

Key words: cobalt, nickel, carbon nanomaterials, bimetallic catalyst, synergistic effect, o-chloronitrobenzene, hydrogenation