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金属有机框架材料HKUST-1对从水溶液中去除天然有机物的吸附性能洞察。

Insights into metal-organic frameworks HKUST-1 adsorption performance for natural organic matter removal from aqueous solution.

作者信息

Ma Xiaoyan, Wang Lei, Wang Hong, Deng Jing, Song Yali, Li Qingsong, Li Xueyan, Dietrich Andrea M

机构信息

College of Civil Engineering, Zhejiang University of Technology, Hangzhou 310023, China.

School of Civil Engineering and Architecture, Zhejiang University of Science and Technology, Hangzhou 310023, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt C):126918. doi: 10.1016/j.jhazmat.2021.126918. Epub 2021 Sep 22.

Abstract

Natural organic matter (NOM) has rich halogenation reactive sites, therefore acts as the main precursor of disinfection byproducts (DBPs) in the chlorine disinfection process during drinking water treatment. In this research, high-quality metal-organic framework HKUST-1 is rapidly synthesized by a solvothermal method, and we are the first to report adsorption of aqueous humic acid (HA), representing NOM, and its adsorption behavior, influencing factors, and recycling capability. The crystalline HKUST-1 possessed a microporous framework with a high 1385 m/g specific surface area, and three-dimensional structure as characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM). 99% removal of 5 mg/L HA was observed at pH 5.8, room temperature, and 0.6 g/L HKUST-1. The maximum capacity was 14.42 mg HA/g HKUST-1 at room temperature. The Langmuir adsorption isotherm, quasi-second-order kinetic model, and thermodynamic parameters accurately describe the spontaneous and disorderly endothermic adsorption of HA by HKUST-1. The desorption regeneration process was accomplished by washing HKUST-1 with NaOH and calcination; it showed that HKUST-1 was viable in three regeneration cycles. The mechanism of HA adsorption by HKUST-1 is electrostatic and synergistic interaction between π-π bonding, and hydrogen bonding. HKUST-1 is a potential treatment strategy to remove NOM.

摘要

天然有机物(NOM)具有丰富的卤化反应位点,因此在饮用水处理的氯消毒过程中充当消毒副产物(DBPs)的主要前体。在本研究中,通过溶剂热法快速合成了高质量的金属有机框架HKUST-1,并且我们首次报道了其对代表NOM的水溶性腐殖酸(HA)的吸附及其吸附行为、影响因素和循环利用能力。通过傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)、扫描电子显微镜(SEM)表征,结晶态的HKUST-1具有微孔框架,比表面积高达1385 m/g,且为三维结构。在pH 5.8、室温及0.6 g/L HKUST-1的条件下,观察到对5 mg/L HA的去除率达99%。室温下最大吸附量为14.42 mg HA/g HKUST-1。Langmuir吸附等温线、准二级动力学模型和热力学参数准确描述了HKUST-1对HA的自发无序吸热吸附。通过用NaOH洗涤和煅烧HKUST-1完成解吸再生过程;结果表明HKUST-1在三个再生循环中均可行。HKUST-1对HA的吸附机制是静电作用以及π-π键和氢键之间的协同相互作用。HKUST-1是一种去除NOM的潜在处理策略。

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