A Novel Method for Synthesizing p-Benzoquinone by Direct Catalytic Oxidation of Benzene with Hydrogen Peroxide over Copper-Doped TS-1

论文摘要

Existing methods for synthesizing p-benzoquinone have drawbacks with respect to environmental protection, production scale, or industrial value. Therefore, it is imperative that a simple and environmentally friendly alternative be developed. The approach that involves preparing p-benzoquinone by the catalytic oxidation of benzene with hydrogen peroxide（H2O2） over copper-modified titanium silicalite-1（Cu/TS-1） has a certain superiority due to its green synthesis and mild reaction conditions. In this study, Cu/TS-1 catalyst was prepared by the wet impregnation of TS-1 with an aqueous solution of Cu（NO3）2 and then characterized by X-ray diffraction, Fourier transform infrared spectroscopy, diffuse reflectance UV–Vis spectroscopy, scanning electron microscopy, inductively coupled plasma mass spectrometry, X-ray fluorescence, and analysis of the N2 adsorption–desorption isotherms. The results reveal that Cu species exist mainly in the form of amorphous Cu O that is well dispersed on the surface of catalysts, with no major change in the molecular sieve framework. After optimizing the reaction conditions, a desirable p-benzoquinone selectivity（88.4%） and benzene conversion（18.3%） were obtained when the doping of Cu in Cu/TS-1 is 1.95 wt%. In addition, Cu/TS-1 can be conveniently regenerated, showing a slight decrease in catalytic capability after initial use, which then stabilizes in subsequent circulations. The satisfactory stability and low cost of synthesizing Cu/TS-1 give this method considerable potential for further industrialization.

论文目录

• Introduction
• Experimental
•   Materials
•   Syntheses of TS-1 and Cu/TS-1
•   Characterization of Catalysts
•   Catalytic Oxidation of Benzene
• Results and Discussion
•   XRD Characterization
•   FT-IR Characterization
•   SEM Characterization
•   N 2 Adsorption–Desorption and XRF Characterization
•   DR UV–Vis Characterization
• Catalytic Activity Tests
•   Infl uence of Copper Content
•   Infl uence of Catalyst Concentration
•   Infl uence of Temperature
•   Infl uence of Reaction Time
•   Infl uence of H 2 O 2:Benzene（Molar Ratio）
•   Infl uence of Solvent
•   Catalyst Circulation
• Conclusions

文章来源

类型: 期刊论文

作者: Chenxiaodong Li,Qingjun Zhang,Aiwu Zeng

来源: Transactions of Tianjin University 2019年05期

年度: 2019

分类: 工程科技Ⅱ辑,工程科技Ⅰ辑

专业: 有机化工

单位: State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology , Tianjin University,Chemical Engineering Research Center , Collaborative Innovative Center of Chemical Science and Engineering,Tianjin

基金: supported by the National Natural Science Foundation of China (No. 21376163)

分类号: TQ244.61

页码: 517-526

总页数: 10

文件大小: 2505K

下载量: 17