高等学校化学学报 ›› 2012, Vol. 33 ›› Issue (09): 2067.doi: 10.3969/j.issn.0251-0790.2012.09.034

• 物理化学 • 上一篇    下一篇

Mo含量对Ni-Mo-B非晶态合金催化剂结构及催化二硝基甲苯加氢性能的影响

闫少伟1,2, 范辉2, 梁川1, 李忠1   

  1. 1. 太原理工大学煤科学与技术教育部和山西省重点实验室, 太原 030024;
    2. 赛鼎工程有限公司技术中心, 太原 030024
  • 收稿日期:2011-11-15 出版日期:2012-09-10 发布日期:2012-08-14
  • 通讯作者: 李忠,男,博士,教授,博导,主要从事工业催化和碳一化学研究.E-mail:lizhong@tyut.edu.cn E-mail:lizhong@tyut.edu.cn
  • 基金资助:

    国家"九七三"计划项目(批准号: 2005CB221204)资助.

Influence of Mo Content on Microstructure and Catalytic Performance of Ni-Mo-B Amorphous Alloy Catalyst for Dinitrotoluene Hydrogenation

YAN Shao-Wei1,2, FAN Hui2, LIANG Chuan1, LI Zhong1   

  1. 1. Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;
    2. Center of Technology, Sedin Engineering Company Limited, Taiyuan 030024, China
  • Received:2011-11-15 Online:2012-09-10 Published:2012-08-14
  • Contact: Zhong Li E-mail:lizhong@tyut.edu.cn

摘要:

采用化学还原法制备Ni-Mo-B非晶态合金催化剂, 研究了Mo含量对二硝基甲苯加氢制备甲苯二胺催化性能的影响. 结果表明, 当Mo含量(摩尔分数)≤6%时, Mo助剂使Ni-B非晶态合金催化剂的催化活性显著提高, 选择性均达到100%. 通过XRD, TEM, DSC, XPS, ICP和H2-TPD技术对催化剂微观结构进行了表征, 结果表明, 随着Mo助剂含量的增加, Ni-Mo-B非晶态合金催化剂中不仅非晶态结构的无序程度增大, 催化剂粒径逐渐由60 nm左右减小至15 nm左右, 而且分布更加均匀, Ni吸附中心的H2吸附强度变弱, 使氢物种更易于在催化剂表面流动并参与反应, 同时Mo助剂还显著提高了催化剂的热稳定性和抗氧化性. 当Mo含量为6%时, Ni-Mo-B非晶态合金催化剂的催化性能最好, 在2 MPa和110℃反应条件下, 二硝基甲苯转化率达99.8%, 甲苯二胺选择性为100%.

关键词: 二硝基甲苯, 甲苯二胺, 非晶态合金催化剂, Ni-B, Mo助剂

Abstract:

A series of amorphous Ni-Mo-B catalyst was prepared by KBH4 reduction for liquid phase dinitrotoluene(DNT) hydrogenation. The results showed that Ni-B catalyst exhibited high activity and selectivity in liquid phase hydrogenation of DNT to diaminotoluene(TDA), the activity of Ni-B catalyst has been enhanced obviously by introduction of Mo, and the selectivity of TDA was 100% when the molar fraction of Mo was smaller and equal to 6%. The characterizations of XRD, DSC, TEM, XPS, ICP and H2-TPD showed that the addition of Mo could enhance the extent of long-range disorder, reduce the particle diameter from 60 nm to 15 nm, weaken the strength of Ni-H bond, improve the thermal stability and antioxidation, which resulted in the increasing activity of Ni-B. when the molar fraction of Mo was 6%, the conversion of DNT and the selectivity of TDA reached 99.8% and 100%, respectively.

Key words: Dinitrotoluene, Diaminotoluene, Amorphous alloy catalyst, Ni-B, Mo modification

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