Geng Fang-Lan, Chi Hai-Yuan, Zhao Hua-Chao, Wan Jin-Quan, Sun Jian
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China.
Institute of Environmental Research at Greater Bay Area, Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou, China.
Front Bioeng Biotechnol. 2023 Jul 28;11:1205911. doi: 10.3389/fbioe.2023.1205911. eCollection 2023.
Fe-based metal-organic frameworks (MOFs) show high activity toward the activation of peroxodisulfate (PDS) for the removal of organic micropollutants (OMPs) in wastewater treatment. However, there is a phenomenon of Fe ion dissolution in the Fe-based MOFs' active PDS system, and the reasons and influencing factors that cause Fe ion dissolution are poorly understood. In this study, we synthesized four types of Fe-based MOFs and confirmed their crystal structure through characterization. All types of Fe-based MOFs were found to activate PDS and form sulfate radicals (SO ), which effectively remove OMPs in wastewater. During the process of Fe-based MOFs activating PDS for CIP removal, activated species, oxidant reagent, and pH negatively impact the stability performance of the MOFs' structure. The coordination bond between Fe atom and O atom can be attacked by water molecules, free radicals, and H, causing damage to the crystal structure of MOFs. Additionally, Fe (II)-MOFs exhibit the best stability performance, due to the enhanced bond energy of the coordination bond in MOFs by the F ligands. This study summarizes the influencing factors of Fe-based MOFs' damage during PDS activation processes, providing new insights for the future development of Fe-based MOFs.
铁基金属有机框架材料(MOFs)在过二硫酸盐(PDS)活化以去除废水处理中的有机微污染物(OMPs)方面表现出高活性。然而,在铁基MOFs的活性PDS体系中存在铁离子溶解现象,且导致铁离子溶解的原因及影响因素尚不清楚。在本研究中,我们合成了四种类型的铁基MOFs,并通过表征确认了它们的晶体结构。发现所有类型的铁基MOFs均能活化PDS并形成硫酸根自由基(SO ),从而有效去除废水中的OMPs。在铁基MOFs活化PDS去除环丙沙星(CIP)的过程中,活性物种、氧化试剂和pH值对MOFs结构的稳定性性能产生负面影响。铁原子与氧原子之间的配位键会受到水分子、自由基和H的攻击,导致MOFs晶体结构受损。此外,由于F配体增强了MOFs中配位键的键能,Fe(II)-MOFs表现出最佳的稳定性性能。本研究总结了PDS活化过程中铁基MOFs损伤的影响因素,为铁基MOFs的未来发展提供了新的见解。