Li Zongchen, Ma Shengjia, Sang Linfeng, Qu Guojuan, Zhang Tao, Xu Bin, Jin Wei, Zhao Yaping
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.
Chemosphere. 2023 Apr;319:138044. doi: 10.1016/j.chemosphere.2023.138044. Epub 2023 Feb 1.
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.
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。