物理化学学报 >> 2012, Vol. 28 >> Issue (01): 170-176.doi: 10.3866/PKU.WHXB201228170

催化和表面科学 上一篇    下一篇

CuO-ZnO-ZrO2的柠檬酸燃烧法制备及其催化CO2加氢合成甲醇的性能

郭晓明1,2, 毛东森2, 卢冠忠1,2, 王嵩2   

  1. 1. 华东理工大学工业催化研究所, 上海 200237;
    2. 上海应用技术学院应用催化研究所, 上海 200235
  • 收稿日期:2011-08-29 修回日期:2011-10-15 发布日期:2011-12-29
  • 通讯作者: 毛东森, 卢冠忠 E-mail:dsmao@sit.edu.cn; gzhlu@ecust.edu.cn
  • 基金资助:

    上海市科委科研项目(08520513600), 上海市教委重点学科建设项目(J51503)和上海应用技术学院科技发展基金(KJ2010-05)资助

Preparation of CuO-ZnO-ZrO2 by Citric Acid Combustion Method and Its Catalytic Property for Methanol Synthesis from CO2 Hydrogenation

GUO Xiao-Ming1,2, MAO Dong-Sen2, LU Guan-Zhong1,2, WANG Song2   

  1. 1. Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, P. R. China;
    2. Research Institute of Applied Catalysis, Shanghai Institute of Technology, Shanghai 200235, P. R. China
  • Received:2011-08-29 Revised:2011-10-15 Published:2011-12-29
  • Contact: MAO Dong-Sen, LU Guan-Zhong E-mail:dsmao@sit.edu.cn; gzhlu@ecust.edu.cn
  • Supported by:

    The project was supported by the Science and Technology Commission of Shanghai Municipality, China (08520513600), Leading Academic Discipline Project of Shanghai Education Committee, China (J51503), and Science and Technology Development Fund of Shanghai Institute of Science and Technology, China (KJ2010-05).

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摘要： 采用柠檬酸燃烧法制备了CuO-ZnO-ZrO2 (CZZ)催化剂, 并将其用于CO2加氢合成甲醇反应. 按推进剂化学原理对燃烧反应进行了分析, 并采用热重-差热分析(TG-DTA)技术记录了其燃烧行为. 采用X射线衍射(XRD)、氮吸附、程序升温还原(TPR)及氧化亚氮(N2O)反应吸附技术对制得的催化剂进行了表征. 结果表明: 柠檬酸燃烧法的燃烧过程比较温和, 燃料用量对催化剂物化和催化性能的影响不大, 并结合燃烧反应的特点进行了解释. 此外, 还对三种燃料(柠檬酸、尿素和甘氨酸)的用量与CZZ性能之间的关系进行了比较, 表明柠檬酸作燃料具有更好的工艺可控性. 柠檬酸燃烧法是一种简单、快速且有效的制备CZZ催化剂的方法.

关键词: 燃烧合成, 柠檬酸, CuO-ZnO-ZrO2, 二氧化碳加氢, 甲醇

Abstract: CuO-ZnO-ZrO2 (CZZ) catalysts for methanol synthesis from CO2 hydrogenation were prepared by a citric acid combustion method. The combustion reactions were analyzed in terms of propellant chemistry and the combustion behavior was recorded by thermo-gravimetric/differential thermal analysis (TG-DTA). The as-prepared CZZ powders were investigated with X-ray diffraction (XRD), N2 adsorption, temperature-programmed reduction (TPR), and reactive N2O adsorption techniques and the catalytic activities were evaluated for methanol synthesis from CO2 hydrogenation. The results show that the influence of citric acid quantity on the physicochemical and catalytic properties of CZZ is subtle, and the reason is related to the characteristics of the combustion reaction. Furthermore, the relationship between the quantity of fuel (citric acid, urea, and glycine) and the properties of the catalysts was determined. The citric acid combustion method exhibits better controllability and it is a simple, fast, and valuable route for the preparation of the CZZ catalyst for methanol synthesis from CO2 hydrogenation.

Key words: Combustion synthesis, Citric acid, CuO-ZnO-ZrO2, CO2 hydrogenation, Methanol