金属-有机骨架材料NH2-MIL-53(Al)对水中双氯芬酸钠的吸附性能

doi:10.7503/cjcu20170378

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (2): 206.doi: 10.7503/cjcu20170378

• 研究论文: 无机化学 • 上一篇下一篇

金属-有机骨架材料NH₂-MIL-53(Al)对水中双氯芬酸钠的吸附性能

王小兵¹, 石秀仪¹, 周星均², 丘秀珍¹, 卢文贯¹()

1. 韶关学院化学与环境工程学院, 韶关 512005
2. 湖南大学化学化工学院, 长沙 410082

收稿日期:2017-06-14 出版日期:2018-02-10 发布日期:2017-12-18
作者简介:联系人简介: 卢文贯, 男, 博士, 教授, 主要从事功能分子与材料的研究. E-mail: lwg@sgu.edu.cn
基金资助:
广东省自然科学基金项目(批准号: 2016A030307048, 2015A030313750)、广东省普通高校特色创新(自然科学类)项目(批准号: 2014KTSCX169)、韶关市科技计划项目(批准号: 210572)和广东省大学生攀登计划项目(批准号: pdjh2016b0458)资助

Adsorption Behavior of Metal-organic Framework NH₂-MIL-53(Al) for Diclofenac Sodium in Aqueous Solution^†

WANG Xiaobing¹, SHI Xiuyi¹, ZHOU Xingjun², QIU Xiuzhen¹, LU Wenguan^1,^*()

1. College of Chemistry and Environmental Engineering, Shaoguan University, Shaoguan 512005, China
2. College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China

Received:2017-06-14 Online:2018-02-10 Published:2017-12-18
Contact: LU Wenguan E-mail:lwg@sgu.edu.cn
Supported by:
† Supported by the Natural Science Foundation of Guangdong Province, China(Nos.2016A030307048, 2015A030313750), the Featured Innovation Projects in Colleges and Universities of Guangdong Province, China(Natural Science)(No.2014KTSCX169), the Science and Technology Projects of Shaoguan City, China(No.2105-72) and the Student “Climbing” Programs of Guangdong Province, China(No.pdjh2016b0458)

摘要/Abstract

摘要：

采用溶剂热法合成了金属-有机骨架材料NH₂-MIL-53(Al), 对活化后的产物进行了粉末X射线衍射(PXRD)、扫描电子显微镜(SEM)及傅里叶变换红外光谱(FTIR)等表征, 研究了其在水溶液中对双氯芬酸钠的吸附性能. 实验结果表明, NH₂-MIL-53(Al)对双氯芬酸钠具有良好的吸附性能, 对5 mg/L的双氯芬酸钠能在40 min内达到吸附平衡, 且吸附动力学结果符合准二级动力学曲线, 利用Langmuir模型和Freundlich模型拟合吸附等温线, 结果表明Langmuir模型拟合效果更好. 循环吸附实验结果表明NH₂-MIL-53(Al)具有良好的重复利用性. 此外, 结合ζ电位测试结果以及pH值对吸附效果的影响, 对可能的吸附机理进行了阐述.

关键词: NH2-MIL-53(Al), 双氯芬酸钠, 吸附性能, 吸附机理

Abstract:

The metal-organic framework(MOF) material of NH₂-MIL-53(Al) was solvothermally synthesized, and characterized by powder X-ray diffraction(PXRD), scanning electron microscopy(SEM) and Fourier transform infrared spectroscopy(FTIR). The adsorption behavior of the as-prepared NH₂-MIL-53(Al) for diclofenac sodium(DCF) was studied in aqueous solution. The experimental results showed that NH₂-MIL-53(Al) had a high adsorption capacity on the target material and reach adsorption equilibrium in 40 min when the concentration of DCF was 5 mg/L. Furthermore, the adsorption kinetics of NH₂-MIL-53(Al) for DCF conformed to the pseudo second-order kinetics model. Langmuir model and Freundlich model were used to fit the adsorption isotherms, and the Langmuir model showed a better fit. The experiment of cyclic adsorption showed that NH₂-MIL-53(Al) had a good recycle performance. Moreover, the possible adsorption mechanism was demonstrated by the combination of ζ potential tests and adsorption effect experiments under different pH values.

Key words: NH2-MIL-53(Al), Diclofenac sodium, Adsorption capacity, Adsorption mechanism

中图分类号:

O611

TrendMD:

王小兵, 石秀仪, 周星均, 丘秀珍, 卢文贯. 金属-有机骨架材料NH₂-MIL-53(Al)对水中双氯芬酸钠的吸附性能. 高等学校化学学报, 2018, 39(2): 206.

WANG Xiaobing, SHI Xiuyi, ZHOU Xingjun, QIU Xiuzhen, LU Wenguan. Adsorption Behavior of Metal-organic Framework NH₂-MIL-53(Al) for Diclofenac Sodium in Aqueous Solution^†. Chem. J. Chinese Universities, 2018, 39(2): 206.

图/表 9

Fig.1 Molecular structure of DCF

Fig.2 Simulated(a) and experimental(b) PXRD patterns(A), SEM image(B) and FTIR spectrum(C) of NH2-MIL-53(Al)

Fig.3 Time profile of DCF adsorption on NH2-MIL-53(Al)(A, B), pseudo-first-order kinetics model(C) and pseudo-second-order kinetics model(D)

Table 1 Kinetic parameters for adsorption of DCF on NH2-MIL-53(Al)

Pseudo-first-order model			Pseudo-second-order kinetics model
R²	q_e/(mg·g^-1)	k₁/min^-1	R²	q_e/(mg·g^-1)	k₂/(g·mg^-1·min^-1)
0.9664	7.360	0.098	0.9985	9.662	0.0221

Fig.4 Adsorption isotherm of DCF on NH2-MIL-53(Al) a. Langmuir isotherm; b. Freundlich isotherm.

Table 2 Parameters of adsorption isotherm derived from the Langmuir and Freundlich models

Langmuir model			Freundlich model
q_max/(mg·g^-1)	b/(L·mg^-1)	R²	K	n	R²
71.3	0.1006	0.962	16.910	3.462	0.933

Fig.5 Reusability of NH2-MIL-53(Al) toward adsorption of DCF

Fig.6 Effects of pH on DCF adsorption(A) and ζ potential of NH2-MIL-53(Al)(B)

Fig.7 Plausible mechanism of DCF adsorption on NH2-MIL-53(Al) at pH<4(A) and 4<pH<7(B)

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金属-有机骨架材料NH₂-MIL-53(Al)对水中双氯芬酸钠的吸附性能

Adsorption Behavior of Metal-organic Framework NH₂-MIL-53(Al) for Diclofenac Sodium in Aqueous Solution^†

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