化工进展 ›› 2016, Vol. 35 ›› Issue (S2): 168-173.DOI: 10.16085/j.issn.1000-6613.2016.s2.028

• 工业催化 • 上一篇    下一篇

Ag/MIL-101催化剂还原对硝基苯酚反应动力学

秦凤祥1, 李凭力1, 黄益平2, 徐义明2, 陆晓咏2, 刘春江1   

  1. 1. 天津大学化工学院, 天津 300072;
    2. 中建安装工程有限公司, 江苏 南京 210023
  • 收稿日期:2016-04-21 修回日期:2016-06-21 出版日期:2016-12-31 发布日期:2016-12-22
  • 通讯作者: 秦凤祥(1987-),男,博士,工程师。E-mail:qinfeng137@163.com。

Kinetic analysis of catalytic reduction of 4-nitrophenol by Ag/MIL-101

QIN Fengxiang1, LI Pingli1, HUANG Yiping2, XU Yiming2, LU Xiaoyong2, LIU Chunjiang1   

  1. 1. School of Chemical Engineering, Tianjin University, Tianjin 300072, China;
    2. China Construction Installation Engineering Co., Ltd., Nanjing 210023, Jiangsu, China
  • Received:2016-04-21 Revised:2016-06-21 Online:2016-12-31 Published:2016-12-22

摘要: 采用双溶剂浸渍法制备得到了粒径为1.9nm±0.6nm高分散性的Ag/MIL-101催化剂。考察了该催化剂在过量NaBH4存在下,还原对硝基苯酚生成对氨基苯酚反应中的催化性能。本文通过研究催化剂浓度、底物浓度和温度对催化活性的影响,获得不同条件下的表观反应速率常数kapp,采用Langmuir-Hinshelwood吸附反应模型对所得动力学数据进行拟合,获得本征反应速率常数k,底物吸附常数K4-NPKBH4,底物吸附焓、熵以及真实活化能EA,k等热力学参数。研究表明,诱导时间t0直接与该反应速率控制步骤的反应速率常数k有关。

关键词: 催化剂载体, 纳米粒子, 反应动力学, 催化机理

Abstract: Highly dispersed and ultrafine Ag/MIL-101 was prepared by double solvent method(DSM).The size of the nanoparticles was about 1.9nm±0.6nm and the total surface area of nanoparticles could be determined precisely.The catalytic activity was investigated by photo-metrically monitoring the reduction of 4-nitrophenol(4-NP) by an excess of NaBH4 in the presence of the nanoparticles.The kinetic data could be modelled to the Langmuir-Hinshelwood equation.The apparent reaction rate,kapp was found to be related to the total surface of the nanoparticles,to the kinetic constant,k,related to the rate-determining step,and to the adsorption constants K4-NP and KBH4 for 4-NP and borohydride,respectively.The activation energy was obtained by fitting kapp obtained at different temperatures.The study also showed that the induction time,t0,is directly related to the reaction rate constant,k,of the controlling step.

Key words: catalyst support, nanoparticles, reaction kinetics, catalytic mechanism

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