Surface modification of MIL-101(Cr) metal-organic framework in tetrahydropyran aqueous solution by radiolytic method

YU Ming; LIU Zepeng; LIU Sha; LI Wanxin; WANG Ziqiang; LI Linfan; LI Jingye

doi:10.11889/j.1000-3436.2022-0098

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Surface modification of MIL-101(Cr) metal-organic framework in tetrahydropyran aqueous solution by radiolytic method

RADIATION CHEMISTRY | 更新时间：2023-09-15

- Surface modification of MIL-101(Cr) metal-organic framework in tetrahydropyran aqueous solution by radiolytic method
- Journal of Radiation Research and Radiation Processing Vol. 41, Issue 1, Pages: 16-23(2023)
- 作者机构：
  
  1.上海师范大学化学与材料科学学院上海 200234
  2.中国科学院上海应用物理研究所上海 201800
  3.南方科技大学深圳 518055
- 作者简介：
  
  YU Ming (male) was born in 1978, and obtained his doctoral degree from Shanghai Institute of Applied Physics, Chinese Academy of Sciences, in 2010
  LI Linfan, professor, E-mail: lilinfan@sinap.ac.cn
- 基金信息：
  
  National Natural Science Foundation of China(11875313;12075153)
- DOI：10.11889/j.1000-3436.2022-0098
  CLC：
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YU Ming, LIU Zepeng, LIU Sha, et al. Surface modification of MIL-101(Cr) metal-organic framework in tetrahydropyran aqueous solution by radiolytic method. [J]. Journal of Radiation Research and Radiation Processing 41(1):16-23(2023)
DOI：

YU Ming, LIU Zepeng, LIU Sha, et al. Surface modification of MIL-101(Cr) metal-organic framework in tetrahydropyran aqueous solution by radiolytic method. [J]. Journal of Radiation Research and Radiation Processing 41(1):16-23(2023) DOI： 10.11889/j.1000-3436.2022-0098.

摘要

金属有机框架的比表面积和表面亲水性的改变常通过改变其中心金属离子和有机配体的类型来重新合成。本文利用辐射法将金属有机框架MIL-101（Cr）在四氢吡喃水溶液中进行表面改性，大量的羟基被引入到表面，有效地提高了材料的表面亲水性，并在不改变中心金属离子和有机配体的情况下大幅提高了材料的比表面积。傅里叶变换红外光谱和X射线光电子能谱证明了四氢吡喃的辐解产物通过共价键结合到材料的表面，X射线衍射谱证明了材料的晶体结构在辐照后仍然保留，比表面积从1 520 m,2,/g大幅增长至3 247 m,2,/g，水接触角从超疏水的156.7°降低至亲水的53.7°。结果表明：辐照下金属有机框架MIL-101（Cr）与四氢吡喃的反应显著提高了材料的比表面积和亲水性。本研究有望将辐射法应用于简单快速改性制备各种性能的金属有机框架。

Abstract

The specific surface area and surface hydrophilicity of metal-organic frameworks can be tailored by changing their central metal ions and organic ligands. In this study, the surface of the metal-organic framework MIL-101(Cr) was modified in an aqueous solution of tetrahydropyran via the radiolytic method. A large number of hydroxyl groups were introduced to the surface of MIL-101(Cr), thereby effectively improving its surface hydrophilicity and substantially increasing its specific surface area without changing its central metal ion and organic ligand. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy demonstrated that the irradiation products of tetrahydropyran were bound to the surface of MIL-101(Cr) through covalent bonding. X-ray diffractometry demonstrated that the crystal structure of the material was retained after irradiation. The specific surface area of MIL-101(Cr) significantly increased, and water contact angle tests indicated that the surface changed from hydrophobic to hydrophilic after modification. These results show that the irradiation reaction of MIL-101(Cr) with tetrahydropyran significantly improves its specific surface area and hydrophilicity. This study provides guidance on the application of the irradiation method to prepare metal-organic frameworks with various properties by simple and rapid modification.

关键词

金属有机框架MIL-101（Cr）四氢吡喃辐解反应表面改性

Keywords

Metal-organic frameworksMIL-101(Cr)TetrahydropyranIrradiation reactionSurface modification

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