Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number ...Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.展开更多
Poly(urea-formaldehyde)(PUF)microcapsules were prepared by in-situ polymerization with four different pro-cesses in this paper.The chemical composition,surface morphology,particle size distribution,and thermal sta-bil...Poly(urea-formaldehyde)(PUF)microcapsules were prepared by in-situ polymerization with four different pro-cesses in this paper.The chemical composition,surface morphology,particle size distribution,and thermal sta-bility were characterized by FTIR,SEM,particle size analyzer,and TGA,respectively.The results demonstrated that the agglomeration of the PUF microcapsules was related to the agglomeration of the emulsion particles caused by the changes of emulsion interface during the shell polymerization.Due to the slow deposition of the shell material,the PUF microcapsules with the core-shell structure prepared by the process with ammonium chloride as the last additive showed good dispersibility with an average diameter of 6.36μm,high core content of 71.3 wt%,and high yield of 61.3 wt%.The PUF microcapsules had good thermal stability below 216?C.The PUF microcapsules could be uniformly dispersed in the epoxy coating in a single form.The epoxy coating with 2 wt%PUF microcapsules showed good self-healing property,and the service life of the coating was about doubled.展开更多
基金financially supported by the National Natural Science Foundation of China(22176059,21777042,and 22076045)the authors would also like to acknowledge support from the Science and Technology Commission of Shanghai Municipality’s Yangfan Special Project(23YF1408400)the Fundamental Research Funds for the Central Universities.
文摘Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.
基金This work was supported by the Jiangsu National Synergetic Innovation Center for Advanced Materials and the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Poly(urea-formaldehyde)(PUF)microcapsules were prepared by in-situ polymerization with four different pro-cesses in this paper.The chemical composition,surface morphology,particle size distribution,and thermal sta-bility were characterized by FTIR,SEM,particle size analyzer,and TGA,respectively.The results demonstrated that the agglomeration of the PUF microcapsules was related to the agglomeration of the emulsion particles caused by the changes of emulsion interface during the shell polymerization.Due to the slow deposition of the shell material,the PUF microcapsules with the core-shell structure prepared by the process with ammonium chloride as the last additive showed good dispersibility with an average diameter of 6.36μm,high core content of 71.3 wt%,and high yield of 61.3 wt%.The PUF microcapsules had good thermal stability below 216?C.The PUF microcapsules could be uniformly dispersed in the epoxy coating in a single form.The epoxy coating with 2 wt%PUF microcapsules showed good self-healing property,and the service life of the coating was about doubled.