水不溶性铝源合成金属有机骨架MIL-53(Al)及其对洛克沙胂的吸附

doi:10.11901/1005.3093.2017.313

材料研究学报

2017, Vol. 31

Issue (7): 495-501 DOI: 10.11901/1005.3093.2017.313

研究论文

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水不溶性铝源合成金属有机骨架MIL-53(Al)及其对洛克沙胂的吸附

侯书亮¹, 卢慧宫¹, 顾逸凡¹, 马小亮¹, 吴一楠¹(

), 王颖²(

), 李风亭¹

1 同济大学环境科学与工程学院污染控制与资源化研究国家重点实验室上海 200092
2 同济大学化学科学与工程学院上海市化学品分析、风险评估与控制重点实验室上海 200092

Conversion of Water-insoluble Aluminum Sources into Metal-organic Framework MIL-53(Al) and its Adsorptive Removal of Roxarsone

Shuliang HOU¹, Huigong LU¹, Yifan GU¹, Xiaoliang MA¹, Yinan WU¹(

), Ying WANG²(

), Fengting LI¹

1 College of Environmental Science and Engineering, State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, 200092, China
2 Department of Chemistry, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 200092, China

引用本文:

侯书亮, 卢慧宫, 顾逸凡, 马小亮, 吴一楠, 王颖, 李风亭. 水不溶性铝源合成金属有机骨架MIL-53(Al)及其对洛克沙胂的吸附[J]. 材料研究学报, 2017, 31(7): 495-501.
Shuliang HOU, Huigong LU, Yifan GU, Xiaoliang MA, Yinan WU, Ying WANG, Fengting LI. Conversion of Water-insoluble Aluminum Sources into Metal-organic Framework MIL-53(Al) and its Adsorptive Removal of Roxarsone[J]. Chinese Journal of Materials Research, 2017, 31(7): 495-501.

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摘要:

以氧化铝、氢氧化铝、勃姆石为水不溶性金属源,用水热法合成了金属有机骨架MIL-53(Al)。使用SEM、XRD、氮气吸附和TGA表征了产物的形貌和结构,并与用传统水溶性硝酸铝合成的MIL-53(Al)对比。结果表明：使用三种水不溶性金属源都能合成典型的金属有机骨架材料MIL-53(Al)。用水热法制备的MIL-53(Al)产物的BET比表面积都在700~1000 m²/g。结果还表明,使用三种水不溶性金属源合成的MIL-53(Al)骨架的柔性(flexibility)与用常规铝硝酸盐合成的MIL-53(Al)不同。使用氧化铝合成的MIL-53(Al)常温下的孔道主要呈现大孔(lp)结构且骨架刚性较强。与使用其他铝源合成的MIL-53(Al)相比,用氧化铝合成的MIL-53(Al)对洛克沙胂有较好的吸附去除效果,吸附过程符合二级动力学模型。

关键词 ：金属有机骨架, MIL-53, 呼吸效应, 洛克沙胂, 吸附

Abstract：

The MIL-53(Al) was prepared by hydrothermal method from water-insoluble aluminum sources: alumina, aluminum hydroxide, boehmite. The products were characterized by SEM, XRD, N₂ sorption and TGA, simultaneously compared with MIL-53(Al) prepared from aluminum nitrate. The results show that the water-insoluble aluminum sources can be good candidates for the synthesis of typical MIL-53(Al), BET surface areas of which are about 700-1000 m²/g. It’s also noticed that there is different framework flexibility of synthesized MIL-53(Al) from water-insoluble and soluble aluminum sources. The framework of MIL-53(Al) prepared from alumina mainly shows large-pore structure and less flexibility. The adsorption behavior of roxarsone on MIL-53(Al) was investigated. MIL-53(Al) prepared from alumina shows better adsorptive performance towards roxarsone. The adsorption of MIL-53(Al) from alumina fits well with secondary dynamic mode.

Key words： metal-organic frameworks MIL-53 breathing effect roxarsone adsorption

收稿日期: 2016-12-20

ZTFLH:

TB34

基金资助:资助项目国家自然科学基金(51203117, 21305046);中央高校基本科研业务费专项(2014KJ007, 2015KJ001)

作者简介:

作者简介侯书亮,男,1993年生,硕士生

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图1 MIL-53(Al)的晶体结构及其骨架呼吸效应示意图

图2 用四种铝源合成的MIL-53(Al)的XRD谱

图3 用四种铝源合成的MIL-53(Al)的SEM照片

图4 用四种铝源合成的MIL-53(Al)的N2吸附-脱附曲线

表1 四种铝源合成的MIL-53(Al)材料的多孔性能

图5 四种铝源合成的MIL-53(Al)材料热失重曲线

图6 用四种铝源合成的MIL-53(Al)材料对ROX的吸附动力学曲线

表2 四种铝源合成的MIL-53(Al)材料吸附ROX动力学拟合参数

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