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用于水中除砷的 Fe/Zr 双金属 MOFs 的简便制备:高容量、快速动力学和良好的可重复使用性。

Facile fabrication of Fe/Zr binary MOFs for arsenic removal in water: High capacity, fast kinetics and good reusability.

机构信息

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science & Engineering, North China Electric Power University, Baoding 071000, China.

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science & Engineering, North China Electric Power University, Baoding 071000, China; Wetland Research Center for Baiyangdian Lake, North China Electric Power University, Baoding 071000, China.

出版信息

J Environ Sci (China). 2023 Jun;128:213-223. doi: 10.1016/j.jes.2022.08.002. Epub 2022 Aug 12.

DOI:10.1016/j.jes.2022.08.002
PMID:36801036
Abstract

A water-stable bimetallic Fe/Zr metal-organic framework [UiO-66(Fe/Zr)] for exceptional decontamination of arsenic in water was fabricated through a facile one-step strategy. The batch adsorption experiments revealed the excellent performances with ultrafast adsorption kinetics due to the synergistic effects of two functional centers and large surface area (498.33 m/g). The absorption capacity of UiO-66(Fe/Zr) for arsenate [As(V)] and arsenite [As(III)] reached as high as 204.1 mg/g and 101.7 mg/g, respectively. Langmuir model was suitable to describe the adsorption behaviors of arsenic on UiO-66(Fe/Zr). The fast kinetics (adsorption equilibrium in 30 min, 10 mg/L As) and pseudo-second-order model implied the strong chemisorption between arsenic ions and UiO-66(Fe/Zr), which was further confirmed by DFT theoretical calculations. The results of FT-IR, XPS analysis and TCLP test demonstrated that arsenic was immobilized on the surface of UiO-66(Fe/Zr) through Fe/Zr-O-As bonds, and the leaching rates of the adsorbed As(III) and As(V) from the spent adsorbent were only 5.6% and 1.4%, respectively. UiO-66(Fe/Zr) can be regenerated for five cycles without obvious removal efficiency decrease. The original arsenic (1.0 mg/L) in lake and tap water was effectively removed in 2.0 hr [99.0% of As(III) and 99.8% of As(V)]. The bimetallic UiO-66(Fe/Zr) has great potentials in water deep purification of arsenic with fast kinetics and high capacity.

摘要

通过简便的一步法策略,制备了一种水稳定的双金属 Fe/Zr 金属有机骨架[UiO-66(Fe/Zr)],用于水中砷的非凡去除。批处理吸附实验表明,由于两个官能团和大表面积(498.33 m/g)的协同作用,具有超快吸附动力学的优异性能。UiO-66(Fe/Zr)对砷酸盐[As(V)]和亚砷酸盐[As(III)]的吸附容量分别高达 204.1 mg/g 和 101.7 mg/g。Langmuir 模型适合描述砷在 UiO-66(Fe/Zr)上的吸附行为。砷在 UiO-66(Fe/Zr)上的快速动力学(吸附平衡在 30 分钟内,10 mg/L As)和准二级模型表明砷离子与 UiO-66(Fe/Zr)之间存在强烈的化学吸附,这进一步通过 DFT 理论计算得到证实。FT-IR、XPS 分析和 TCLP 测试的结果表明,砷通过 Fe/Zr-O-As 键固定在 UiO-66(Fe/Zr)的表面上,从失活吸附剂中浸出的吸附 As(III)和 As(V)的速率分别仅为 5.6%和 1.4%。UiO-66(Fe/Zr)可以在不降低去除效率的情况下再生五次。在 2.0 小时内,有效去除了湖泊和自来水中的原始砷(1.0 mg/L)[99.0%的 As(III)和 99.8%的 As(V)]。双金属 UiO-66(Fe/Zr)具有快速动力学和高容量,在砷的水深度净化方面具有很大的潜力。

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