Hierarchical Porous Bimetallic FeMn Metal–Organic Framework Gel for Efficient Activation of Peracetic Acid in Antibiotic Degradation

IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL ACS Environmental Au Pub Date : 2023-12-05 DOI:10.1021/acsenvironau.3c00041
Lu Zheng, Jiarui Fu, Baolv Hua, Yi-nan Wu, Yifan Gu, Nianqiao Qin and Fengting Li*, 
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Abstract

Effective techniques for eliminating antibiotics from water environments are in high demand. The peracetic acid (PAA)-based advanced oxidation process has recently drawn increasing attention for its effective antibiotic degrading capability. However, current applications of PAA-based techniques are limited and tend to have unsatisfactory performance. An additional catalyst for PAA activation could provide a promising solution to improve the performance of PAA. Bulky metal–organic framework gels (MOGs) stand out as ideal catalysts for PAA activation owing to their multiple advantages, including large surface areas, high porosity, and hierarchical pore systems. Herein, a bimetallic hierarchical porous structure, i.e., FeMn13BTC, was synthesized through a facile one-pot synthesis method and employed for PAA activation in ofloxacin (OFX) degradation. The optimized FeMn MOG/PAA system exhibited efficient catalytic performance, characterized by 81.85% OFX degradation achieved within 1 h owing to the specific hierarchical structure and synergistic effect between Fe and Mn ions, which greatly exceeded the performance of the only PAA-catalyzed system. Furthermore, the FeMn MOG/PAA system maintained >80% OFX degradation in natural water. Quenching experiments, electron spin resonance spectra, and model molecular degradation revealed that the primary reactive oxygen species responsible for the catalytic effect was R–O, especially CH3C(═O)OO, with minor contributions of OH and 1O2. Overall, introduction of the MOG catalyst strategy for PAA activation achieved high antibiotic degradation performance, establishing a paradigm for the design of heterogeneous hierarchical systems to broaden the scope of catalyzed water treatment applications.

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在抗生素降解过程中高效活化过乙酸的分层多孔双金属铁锰金属有机框架凝胶
消除水环境中抗生素的有效技术需求量很大。最近,基于过乙酸(PAA)的高级氧化工艺因其有效的抗生素降解能力而受到越来越多的关注。然而,目前基于 PAA 的技术应用有限,性能往往不尽如人意。为 PAA 的活化添加催化剂可为改善 PAA 的性能提供一种前景广阔的解决方案。大块金属有机框架凝胶(MOGs)具有大表面积、高孔隙率和分层孔隙体系等多种优点,是 PAA 活化的理想催化剂。本文通过简单的一锅合成法合成了一种双金属分层多孔结构,即 FeMn13BTC,并将其用于氧氟沙星(OFX)降解过程中的 PAA 活化。优化后的 FeMn MOG/PAA 体系表现出高效的催化性能,由于其特殊的分层结构以及铁离子和锰离子之间的协同效应,在 1 h 内实现了 81.85% 的 OFX 降解,大大超过了仅有的 PAA 催化体系。此外,FeMn MOG/PAA 系统还能在天然水中保持 80% 的 OFX 降解率。淬灭实验、电子自旋共振光谱和模型分子降解显示,产生催化效果的主要活性氧是 R-O-,尤其是 CH3C(═O)OO-,其次是 -OH 和 1O2。总之,采用 MOG 催化剂活化 PAA 的策略实现了较高的抗生素降解性能,为设计异构分层体系建立了范例,从而拓宽了催化水处理的应用范围。
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ACS Environmental Au
ACS Environmental Au 环境科学-
CiteScore
7.10
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0.00%
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0
期刊介绍: ACS Environmental Au is an open access journal which publishes experimental research and theoretical results in all aspects of environmental science and technology both pure and applied. Short letters comprehensive articles reviews and perspectives are welcome in the following areas:Alternative EnergyAnthropogenic Impacts on Atmosphere Soil or WaterBiogeochemical CyclingBiomass or Wastes as ResourcesContaminants in Aquatic and Terrestrial EnvironmentsEnvironmental Data ScienceEcotoxicology and Public HealthEnergy and ClimateEnvironmental Modeling Processes and Measurement Methods and TechnologiesEnvironmental Nanotechnology and BiotechnologyGreen ChemistryGreen Manufacturing and EngineeringRisk assessment Regulatory Frameworks and Life-Cycle AssessmentsTreatment and Resource Recovery and Waste Management
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