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使用锆-二茂铁金属有机框架材料与过一硫酸盐联用从水中强化去除亚砷酸盐:氧化及多位点吸附机制

Enhanced arsenite removal from water using zirconium-ferrocene MOFs coupled with peroxymonosulfate:oxidation and multi-sites adsorption mechanism.

作者信息

Li Zongchen, Ma Shengjia, Sang Linfeng, Qu Guojuan, Zhang Tao, Xu Bin, Jin Wei, Zhao Yaping

机构信息

Shanghai Engineering Research Center of Biotransformation of Organic Solid Waste, Technology Innovation Center for Land Spatial Eco-restoration in Metropolitan Area of Ministry of Natural Resources, Shanghai Key Laboratory for Urban Ecological Process and Eco-Restoration, Institute of Eco-Chongming and School of Ecological and Environmental Sciences, East China Normal University, Shanghai, 200241, China; School of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China.

Shanghai Engineering Research Center of Biotransformation of Organic Solid Waste, Technology Innovation Center for Land Spatial Eco-restoration in Metropolitan Area of Ministry of Natural Resources, Shanghai Key Laboratory for Urban Ecological Process and Eco-Restoration, Institute of Eco-Chongming and School of Ecological and Environmental Sciences, East China Normal University, Shanghai, 200241, China.

出版信息

Chemosphere. 2023 Apr;319:138044. doi: 10.1016/j.chemosphere.2023.138044. Epub 2023 Feb 1.

Abstract

The efficient removal of arsenite (As(III)) poses a significant challenge to traditional water treatment technologies due to its high toxicity and mobility. In this work, multifunctional Zirconium-Ferrocene Metal Organic Framework (ZrFc-MOF) fabricated with redox-active 1,1-ferrocene dicarboxylic acid ligands and Zr precursors were elaborated to achieve remarkably enhanced As(III) removal via activation by peroxymonosulfate (PMS). The adsorption affinity coefficient increased from 0.097 to 2.035 L mg and the maximum adsorption capacity increased from 59.79 to 111.34 mg g compared with that without PMS. Besides the conventional homogeneous PMS oxidation and the following adsorption through Zr-O clusters of ZrFc-MOFs, the enhanced As(III) removal synergistic combines the oxidation mechanism of As(III) by reactive oxygen species (•OH, SO, O and O) formed in Ferrocene (Fc) activating PMS process with the simultaneous formed extra adsorption sites of Ferrocenium (Fc). PMS also help ZrFc-MOF to avoid destruction in harsh alkaline condition, making the effluent in this advanced treatment meet the World Health Organization (WHO) threshold of 10 μg L over a wide range of initial pH (2-11) with high selectivity and durability. These results indicate that this novel Fc-based MOFs activating PMS system has potential applicability for As(III) in oxidation and selectively capturing in the water environment.

摘要

由于亚砷酸盐(As(III))具有高毒性和高迁移性,其有效去除对传统水处理技术构成了重大挑战。在本研究中,我们制备了由具有氧化还原活性的1,1-二茂铁二甲酸配体和锆前驱体制备的多功能锆-二茂铁金属有机框架(ZrFc-MOF),以通过过一硫酸盐(PMS)活化实现显著增强的As(III)去除效果。与未添加PMS的情况相比,吸附亲和系数从0.097增加到2.035 L mg,最大吸附容量从59.79增加到111.34 mg g。除了传统的均相PMS氧化以及随后通过ZrFc-MOFs的Zr-O簇进行的吸附外,增强的As(III)去除效果还将二茂铁(Fc)活化PMS过程中形成的活性氧物种(•OH、SO、O和O)对As(III)的氧化机制与同时形成的二茂铁鎓(Fc)额外吸附位点协同结合。PMS还帮助ZrFc-MOF在苛刻的碱性条件下避免破坏,使得在广泛的初始pH值(2-11)范围内,该深度处理的出水符合世界卫生组织(WHO)规定的10 μg L阈值,具有高选择性和耐久性。这些结果表明,这种基于二茂铁的新型MOFs活化PMS系统在水环境中对As(III)的氧化和选择性捕获方面具有潜在的应用价值。

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