高稳定性的含氟多级孔共价有机框架材料

doi:10.7503/cjcu20180190

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (11): 2357.doi: 10.7503/cjcu20180190

高稳定性的含氟多级孔共价有机框架材料

陈奇丹¹, 唐俊杰^1,², 方千荣^1,²()

1. 吉林大学珠海学院, 珠海 519041
2. 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012

收稿日期:2017-03-12 出版日期:2018-11-10 发布日期:2018-08-03
作者简介:联系人简介: 方千荣, 男, 博士, 教授, 博士生导师, 主要从事多孔晶体材料的定向合成和性能研究. E-mail: qrfang@jlu.edu.cn
基金资助:
国家自然科学基金(批准号: 21571079)和吉林大学珠海学院创新能力培育工程项目(批准号: 2017XJCQ006)资助.

Highly Stable Fluorine Containing Hierarchical Porous Covalent Organic Framework^†

CHEN Qidan¹, TANG Junjie^1,², FANG Qianrong^1,^2,^*()

1. Zhuhai College of Jilin University, Zhuhai 519041, China
2. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun 130012, China

Received:2017-03-12 Online:2018-11-10 Published:2018-08-03
Contact: FANG Qianrong E-mail:qrfang@jlu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.21571079) and the Zhuhai College Innovation Capacity Cultivation Project of Jilin University, China(No. 2017XJCQ006).

摘要/Abstract

摘要：

设计合成了一种新型含氟原子双孔共价有机框架(COF)——四(4-氨基苯)乙烯-2,3,5,6-四氟对二苯甲醛-COF(ETTA-TFA-COF), ETTA-TFA-COF是由1个D_2h对称单体和1个C₂对称单体连接而成的六角星形状结构, 具有2.93 nm六边形与1.43 nm三角形的双孔结构. 通过理论模拟、粉末X射线衍射(PXRD)、氮气吸附-解吸表征和傅里叶变换红外光谱(FTIR)等证实了ETTA-TFA-COF的结构. 同时, 通过与结构相似但不含氟原子的COF材料对比发现, ETTA-TFA-COF材料在碱性溶液中展现出优异的稳定性.

关键词: 共价有机框架, 含氟多孔材料, 晶体结构, 选择性吸附

Abstract:

Covalent organic frameworks(COFs) are an emerging class of crystalline and porous polymers synthesized by condensation reactions of organic building blocks linked through strong covalent bonds. How-ever, constructing dual-pore COFs with applicative building blocks were faced with enormous challenges due to the complicated topological structures formed through the limited strategies. Herein we describe the design and synthesis of a new dual-pore COF with a hexagram-like structure, named ETTA-TFA-COF, synthesized by linking a D_2h symmetric monomer and a C₂ symmetric monomer which leading the formation of dual-pore structure. The structure of the ETTA-TFA-COF was confirmed by theoretical simulation, powder X-ray diffraction(PXRD) investigation, nitrogen adsorption-desorption study, and FTIR spectra analysis. In the meantime, ETTA-TFA-COF material exhibit excellent stability in alkaline solution compared to COF materials of similar structure but without fluorine atoms.

Key words: Covalent organic frameworks, Fluorine containing hierarchical porous material, Crystal structure, Selective adsorption

中图分类号:

O611.4

TrendMD:

陈奇丹, 唐俊杰, 方千荣. 高稳定性的含氟多级孔共价有机框架材料. 高等学校化学学报, 2018, 39(11): 2357.

CHEN Qidan, TANG Junjie, FANG Qianrong. Highly Stable Fluorine Containing Hierarchical Porous Covalent Organic Framework^†. Chem. J. Chinese Universities, 2018, 39(11): 2357.

图/表 8

Scheme 1 Synthesis and schematic representation of the simulated structure of ETTA-TFA-COFC: gray; N: blue; F: turquoise; H atoms are omitted for clarity.

Fig.1 Possible structures modelling predicted by accelrys Material Studio 7.0 software package (A) AA-H structure; (B) AA-O structure; (C) AB-H structure; (D) AB-O structure.C: gray, N: blue, F: turquoise; H atoms are omitted for clarity.

Fig.2 PXRD patterns of ETTA-TFA-COFa. Experimental; b. refined; c. diffe-rence of plot between the experimental and refined PXRD patterns; d. simulated PXRD pattern for AA-H structure; e. AB-H structure; f. AA-O structure; g. AB-O structure. Inset: detailed patterns for experimental(red) and simulated AA-H structure.

Fig.3 FTIR spectra of ETTA-TFA-COF(a), ETTA(b) and TFA(c)

Fig.4 TGA curve of ETTA-TFA-COF

Fig.5 SEM(A) and TEM(B) images of ETTA-TFA-COF

Fig.6 N2 adsorption-desorption isotherms(A) and pore-size distribution(B) of ETTA-TFA-COFAdsorption and desorption points are represented by filled and empty symbols, respectively.

Fig.7 XRD patterns of ETTA-PA-COF(A) and ETTA-TFA-COF(B) after treatment with different alkaline solutions for 24 ha. H2O; b. 3 mol/L NaOH solution; c. 6 mol/L NaOH solution; d. 9 mol/L NaOH solution.

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高稳定性的含氟多级孔共价有机框架材料

Highly Stable Fluorine Containing Hierarchical Porous Covalent Organic Framework^†

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高稳定性的含氟多级孔共价有机框架材料

Highly Stable Fluorine Containing Hierarchical Porous Covalent Organic Framework†

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Highly Stable Fluorine Containing Hierarchical Porous Covalent Organic Framework^†