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磁性可回收光芬顿催化剂 ZnFeO@MIL-88A(Fe) 的巧妙构建及其对左氧氟沙星的吸附降解活性。

Ingenious construction of a magnetic-recyclable photo-Fenton catalyst ZnFeO@MIL-88A(Fe) and its adsorption-degradation activity toward levofloxacin.

机构信息

Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua 321004, China.

Jinhua Customs Comprehensive Technology Service Center, Jinhua 321004, China.

出版信息

J Environ Sci (China). 2025 May;151:677-691. doi: 10.1016/j.jes.2024.04.043. Epub 2024 May 7.

DOI:10.1016/j.jes.2024.04.043
Abstract

Monotonic pore size and particles inseparability of metal-organic frameworks (MOFs) caused serious effects on its light absorption ability and charge separation, restricting its application for antibiotic such as levofloxacin (LEV) degradation in water. In this study, a magnetically detachable nano-photocatalyst (ZnFeO@MIL-88A(Fe)) was synthesized using a simple two-step hydrothermal technique. The morphology and microstructure analyses showed that n-type ZnFeO catalyst particles were efficiently assembled onto the surface of MIL-88A(Fe) crystal. Photocatalytic activity studies indicated that the ZnFeO@MIL-88A(Fe) plus HO exhibiting a significantly boosted photo-Fenton activity toward LEV at visible light irradiation, compared to the pure ZnFeO and MIL-88A(Fe), the degradation efficiency accordingly reached up to nearly 82% and 25% within 60 min. This excellent photocatalytic performance was ascribed to the synergistic effects of the heterogeneous structure of ZnFeO and MIL-88A(Fe), whereby the efficient separation of charge carriers in the catalytic system is mutually reinforced with the efficient reduction of Fe and Fe. Meanwhile, the degradation mechanism and intermediates of LEV during the photo-Fenton reaction process were also studied in depth through free radical burst, electron paramagnetic resonance, and mass spectrometry analyses, etc. Additionally, the ZnFeO@MIL-88A(Fe) composite catalyst displayed significant stability and ease of separation, indicating potential for the photo-oxidative degradation of organic pollutants.

摘要

金属有机骨架(MOFs)的单分散孔径和颗粒不可分离性对其光吸收能力和电荷分离产生了严重影响,限制了其在水中抗生素如左氧氟沙星(LEV)降解方面的应用。在这项研究中,采用简单的两步水热技术合成了一种可磁分离的纳米光催化剂(ZnFeO@MIL-88A(Fe))。形貌和微观结构分析表明,n 型 ZnFeO 催化剂颗粒有效地组装到 MIL-88A(Fe)晶体表面。光催化活性研究表明,与纯 ZnFeO 和 MIL-88A(Fe)相比,ZnFeO@MIL-88A(Fe)加 HO 在可见光照射下对 LEV 表现出显著增强的光芬顿活性,降解效率在 60 分钟内分别达到近 82%和 25%。这种优异的光催化性能归因于 ZnFeO 和 MIL-88A(Fe)的异质结构的协同作用,其中催化体系中载流子的有效分离与 Fe 和 Fe 的有效还原相互增强。同时,还通过自由基爆发、电子顺磁共振和质谱分析等方法深入研究了光芬顿反应过程中 LEV 的降解机制和中间产物。此外,ZnFeO@MIL-88A(Fe)复合催化剂表现出显著的稳定性和易于分离性,表明其在有机污染物的光氧化降解方面具有潜在应用价值。

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