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使用 Fe-MOF 作为微反应器制备高质量的 Al@Fe-MOF 以提高亚硒酸盐的吸附性能。

High-quality Al@Fe-MOF prepared using Fe-MOF as a micro-reactor to improve adsorption performance for selenite.

机构信息

Department of Chemistry and Environmental Engineering, Hubei University for Nationalities, Enshi, 445000, China.

Department of Chemistry and Environmental Engineering, Hubei University for Nationalities, Enshi, 445000, China.

出版信息

J Hazard Mater. 2019 Feb 15;364:272-280. doi: 10.1016/j.jhazmat.2018.10.030. Epub 2018 Oct 16.

DOI:10.1016/j.jhazmat.2018.10.030
PMID:30384236
Abstract

High-quality Al@Fe-MOF was prepared by in situ modification of Fe-MOF with Al to improve the adsorption performance for selenite (Se(Ⅳ)). The structures and properties of Al@Fe-MOF were characterized by powder X-ray diffraction, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS), nitrogen isothermal adsorption-desorption measurement and zeta potential. The adsorption performance of Al@Fe-MOF for Se(Ⅳ) was studied by batch adsorption experiments. A large number of pores in Al@Fe-MOF were filled by AlOOH and some bayerite formed on the surfaces. Compared with those of Fe-MOF, the specific surface area (SSA) and microporosity of Al@Fe-MOF decreased to 1368 m/g and 38.5%, respectively. Hydrolysis occurred at pH > 5.0 for Fe-MOF, but did not for Al@Fe-MOF at the pH range of 3.0-7.0. Compared with in Fe-MOF, the adsorption capacity and efficiency of SSA for Se(Ⅳ) were increased by 77% and 112%, and the average free energy of adsorption was increased to 11.62 kJ/mol in Al@Fe-MOF. Besides, the Se(Ⅳ) adsorption amount of Al@Fe-MOF was almost not influenced by the pH from 3.0 to 7.0. The high resolution XPS (HR-XPS) and pH analysis indicated that Al species in Al@Fe-MOF could significantly increase the density of adsorption sites to improve its adsorption capacity for Se(Ⅳ).

摘要

通过原位修饰 Fe-MOF 用 Al 制备了高质量的 Al@Fe-MOF,以提高其对亚硒酸盐(Se(Ⅳ))的吸附性能。采用粉末 X 射线衍射、高分辨率透射电子显微镜、X 射线光电子能谱(XPS)、氮气等温吸附-脱附测量和动电电位对 Al@Fe-MOF 的结构和性质进行了表征。通过批量吸附实验研究了 Al@Fe-MOF 对 Se(Ⅳ)的吸附性能。Al@Fe-MOF 中的大量孔被 AlOOH 填充,表面形成了一些拜耳石。与 Fe-MOF 相比,Al@Fe-MOF 的比表面积(SSA)和微孔体积分别降低至 1368 m/g 和 38.5%。Fe-MOF 在 pH > 5.0 时发生水解,但在 3.0-7.0 pH 范围内的 Al@Fe-MOF 不会发生水解。与 Fe-MOF 相比,Al@Fe-MOF 对 Se(Ⅳ)的吸附容量和 SSA 效率分别提高了 77%和 112%,平均吸附自由能增加到 11.62 kJ/mol。此外,Al@Fe-MOF 的 Se(Ⅳ)吸附量几乎不受 3.0-7.0 pH 的影响。高分辨率 XPS(HR-XPS)和 pH 分析表明,Al@Fe-MOF 中的 Al 物种可以显著增加吸附位点的密度,从而提高其对 Se(Ⅳ)的吸附能力。

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