化工学报 ›› 2020, Vol. 71 ›› Issue (1): 283-289.DOI: 10.11949/0438-1157.20191213

• 催化、动力学与反应器 • 上一篇    下一篇

钛基金属-有机框架材料的改性及其催化性能研究

曲云鹏1,2(),张丙兴1,2,石金彪1,2,谭秀娘1,2,韩布兴1,2,杨冠英1,张建玲1,2()   

  1. 1. 中国科学院化学研究所,北京 100190
    2. 中国科学院大学化学科学学院,北京 100049
  • 收稿日期:2019-10-23 修回日期:2019-11-07 出版日期:2020-01-05 发布日期:2020-01-05
  • 通讯作者: 张建玲
  • 作者简介:曲云鹏(1997—),男,学士,quyunpeng15@mails.ucas.ac.cn
  • 基金资助:
    国家自然科学基金项目(21525316)

Study on modification of titanium-based metal-organic framework and catalytic performance

Yunpeng QU1,2(),Bingxing ZHANG1,2,Jinbiao SHI1,2,Xiuniang TAN1,2,Buxing HAN1,2,Guanying YANG1,Jianling ZHANG1,2()   

  1. 1. Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    2. School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100190, China
  • Received:2019-10-23 Revised:2019-11-07 Online:2020-01-05 Published:2020-01-05
  • Contact: Jianling ZHANG

摘要:

使用双氧水在一定温度下对钛基金属-有机框架材料NH2-MIL-125进行改性处理,制备得到一系列材料,系统地研究了改性方法及改性条件对材料性能的影响。结果表明,经改性处理后的材料,在可见光催化苯甲醇氧化反应中的催化速率有显著提高;同时,改性过程中的双氧水用量及改性温度对材料的结构、性质和光催化性能都有十分重要的影响。当双氧水为10 ml、改性温度为50℃时,改性材料具有优异的催化活性、选择性以及良好的稳定性,其催化速率与NH2-MIL-125相比提高近6倍。

关键词: 金属-有机框架, NH2-MIL-125, 催化剂, 光化学, 氧化

Abstract:

A series of materials were prepared by modifying titanium based metal-organic framework material NH2-MIL-125 with hydrogen peroxide at a certain temperature. The effects of modification methods and conditions on the properties of materials were studied systematically. However, NH2-MIL-125 as a photocatalyst suffers from low catalytic activity and stability, which largely restrict its practical applications. In order to improve the catalytic activity of NH2-MIL-125, a solvothermal route by using H2O2 was used to modify NH2-MIL-125. A series of materials were synthesized by treating NH2-MIL-125 with different volumes of H2O2 at different temperatures. X-ray diffraction, scanning electron microscope, transmission electron microscope, ultraviolet-visible light absorption spectroscopy, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy and N2 adsorption analysis were used to characterize the structures and properties of the obtained product. Furthermore, their photocatalytic performances for the visible-light-driven oxidation of benzyl alcohol were tested. The results show that the product modified by 10 ml H2O2 at 50℃ exhibits excellent catalytic activity and selectivity. The maximum turnover frequency is nearly 6 times as high as that of NH2-MIL-125 at the same experimental conditions. The partial loss of organic ligands and the introduction of peroxide groups could generate more catalytic-active sites, which is responsible for the improved catalytic activity.

Key words: metal-organic framework, NH2-MIL-125, catalyst, photochemistry, oxidation

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