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利用共价有机框架壳对磁芯进行表面保护的方法及其在酸性废水中深度去除 As(III)中的应用。

Surface protection method for the magnetic core using covalent organic framework shells and its application in As(III) depth removal from acid wastewater.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

出版信息

J Environ Sci (China). 2022 May;115:1-9. doi: 10.1016/j.jes.2021.07.017. Epub 2021 Aug 1.

Abstract

FeO-based materials are widely used for magnetic separation from wastewater. However, they often suffer from Fe-leaching behavior under acidic conditions, decreasing their activity and limiting sustainable practical applications. In this study, covalent organic frameworks (COFs) were used as the shell to protect the FeO core, and the FeO@COF core-shell composites were synthesized for As(III) removal from acid wastewater. The imine-linked COFs can in situ grow on the surface of the FeO core layer by layer with [COFs/FeO] ratio of up to 2:1. The Fe-leaching behavior was weakened over a wide pH range of 1-13. Moreover, such composites keep their magnetic characteristic, making them favorable for nanomaterial separation. As(III) batch adsorption experiments results indicated that, when COFs are used as the shell for the FeO core, a balance between As(III) removal efficiencies and the thickness of the COF shell exists. Higher As(III) removal efficiencies are obtained when the [COFs/FeO] ratios were < 1.5:1, but thicker COF shells were not beneficial for As(III) removal. Such composites also exhibited better As(III) removal performances in the pH range of 1-7. Over a wide pH range, the zeta potential of FeO@COF core-shell composites becomes more positive, which benefits the capture of negative arsenic ions. In addition, thinner surface COFs were favorable for mass transfer and facilitating the reaction of Fe and As elements. Our study highlights the promise of using COFs in nanomaterial surface protection and achieving As(III) depth removal under acidic conditions.

摘要

基于 FeO 的材料广泛用于从废水中进行磁性分离。然而,它们在酸性条件下经常遭受 Fe 浸出行为,降低了它们的活性并限制了可持续的实际应用。在这项研究中,共价有机框架(COFs)被用作保护 FeO 核的壳,合成了 FeO@COF 核壳复合材料,用于从酸性废水中去除 As(III)。亚胺键合的 COFs 可以通过层层自组装在 FeO 核层表面原位生长,达到 [COFs/FeO] 比高达 2:1。Fe 浸出行为在 pH 值为 1-13 的宽范围内减弱。此外,这些复合材料保持其磁性特征,有利于纳米材料分离。As(III)批吸附实验结果表明,当 COFs 用作 FeO 核的壳时,存在去除效率和 COF 壳厚度之间的平衡。当 [COFs/FeO] 比 <1.5:1 时,获得了更高的 As(III)去除效率,但更厚的 COF 壳不利于 As(III)去除。这些复合材料在 pH 值为 1-7 的范围内也表现出更好的 As(III)去除性能。在宽 pH 范围内,FeO@COF 核壳复合材料的动电位变得更正,有利于捕获负砷离子。此外,更薄的表面 COFs 有利于传质并促进 Fe 和 As 元素的反应。我们的研究强调了在纳米材料表面保护中使用 COFs 并在酸性条件下实现 As(III)深度去除的前景。

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