Lu Zheng, Jiarui Fu, Baolv Hua, Yi-nan Wu, Yifan Gu, Nianqiao Qin and Fengting Li*,
{"title":"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","authors":"Lu Zheng, Jiarui Fu, Baolv Hua, Yi-nan Wu, Yifan Gu, Nianqiao Qin and Fengting Li*, ","doi":"10.1021/acsenvironau.3c00041","DOIUrl":null,"url":null,"abstract":"<p >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<sup>•</sup>, especially CH<sub>3</sub>C(═O)OO<sup>•</sup>, with minor contributions of <sup>•</sup>OH and <sup>1</sup>O<sub>2</sub>. 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.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 2","pages":"56–68"},"PeriodicalIF":6.7000,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00041","citationCount":"0","resultStr":"{\"title\":\"Hierarchical Porous Bimetallic FeMn Metal–Organic Framework Gel for Efficient Activation of Peracetic Acid in Antibiotic Degradation\",\"authors\":\"Lu Zheng, Jiarui Fu, Baolv Hua, Yi-nan Wu, Yifan Gu, Nianqiao Qin and Fengting Li*, \",\"doi\":\"10.1021/acsenvironau.3c00041\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >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<sup>•</sup>, especially CH<sub>3</sub>C(═O)OO<sup>•</sup>, with minor contributions of <sup>•</sup>OH and <sup>1</sup>O<sub>2</sub>. 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.</p>\",\"PeriodicalId\":29801,\"journal\":{\"name\":\"ACS Environmental Au\",\"volume\":\"4 2\",\"pages\":\"56–68\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2023-12-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00041\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Environmental Au\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsenvironau.3c00041\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Environmental Au","FirstCategoryId":"1085","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsenvironau.3c00041","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Hierarchical Porous Bimetallic FeMn Metal–Organic Framework Gel for Efficient Activation of Peracetic Acid in Antibiotic Degradation
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.
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