The current modified electro-Fenton system was designed to develop a more convenient and efficient undivided system for practical wastewater treatment. The system adopted a cathode portion that employed magnetic stirr...The current modified electro-Fenton system was designed to develop a more convenient and efficient undivided system for practical wastewater treatment. The system adopted a cathode portion that employed magnetic stirring instead of common oxygen gas diffusion or gas sparging to supply oxygen gas for the electrolyte solution. Key factors influencing the cathode fabrication and activit） were investigated. The degradation of acid fuchsine with a self-made graphite-polytetrafluorethylene cathode was studied using spectrophotometer. It was found that the cathode generated hydrogen peroxide with high current efficiency and the hydrogen peroxide yield of the cathode did not decay after 10 times reuse. With the Pt anode at a ferrous ion concentration of 0.5 mmol/L, a pH of 3, and using magnetic stirring, dye decolorization could be rapidly accomplished but the destruction of benzene rings and intermediates was fairly difficult. With a Fe anode, dye degradation was more complete.展开更多
A novel plasmonic photo‐Fenton catalyst of Ag/AgCl/Fe‐S was synthesized by ion exchange and photoreduction methods.The obtained catalyst was characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,scan...A novel plasmonic photo‐Fenton catalyst of Ag/AgCl/Fe‐S was synthesized by ion exchange and photoreduction methods.The obtained catalyst was characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,scanning electron microscope imaging,and Brunauer‐Emmett‐Teller measurements.Moreover,the photocatalytic activity of Ag/AgCl/Fe‐S was investigated for its degradation activity towards bisphenol A(BPA)as target pollutant under visible light irradiation.The effects of H2O2concentration,pH value,illumination intensity,and catalyst dosage on BPA degradation were examined.Our results indicated that the Ag/AgCl material was successfully loaded onto Fe‐sepiolite and showed a high photocatalytic activity under illumination by visible light.Furthermore,active species capture experiments were performed to explore the photocatalytic mechanism of the Ag/AgCl/Fe‐S in this heterogeneous photo‐Fenton process,where the major active species included hydroxyl radicals(?OH)and holes(h+).展开更多
The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this probl...The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this problem.The original Fenton system relies on the hydroxyl radicals produced by Fe(Ⅱ)/H_(2)O_(2) to oxidize the organic contaminants.However,the application of the Fenton system is limited by its low iron cycling efficiency and the high risks of hydrogen peroxide transportation and storage.The introduction of external energy(including light and electricity etc.)can effectively promote the Fe(Ⅲ)/Fe(Ⅱ)cycle and the reduction of oxygen to produce hydrogen peroxide in situ.This review introduces three in-situ Fenton systems,which are electro-Fenton,Photo-Fenton,and chemical reaction.The mechanism,influencing factors,and catalysts of these three in-situ Fenton systems in degrading EOCs are discussed systematically.This review strengthens the understanding of Fenton and in-situ Fenton systems in degradation,offering further insight into the real application of the in-situ Fenton system in the removal of EOCs.展开更多
Under visible light illumination,2,3-diaminophenazine(DAPN)was generated from the oxidation of o-phenylenediamine(OPDA)in Fe^3+/H2O2 solution.Hydroxyl radical(*OH)produced in this system was determined by directly mea...Under visible light illumination,2,3-diaminophenazine(DAPN)was generated from the oxidation of o-phenylenediamine(OPDA)in Fe^3+/H2O2 solution.Hydroxyl radical(*OH)produced in this system was determined by directly measuring the concentration of DAPN.In comparison with the traditional methods,the determination is more accurate and simple.展开更多
本文以辽河油田沈阳采油厂某采油作业区石油污染土壤为研究对象,探究H2O2浓度、FeSO4浓度、反应体系pH、水土比、反应时间等因素对石油污染土壤中石油烃降解效果的影响。研究结果表明,H2O2投加浓度对石油烃的降解效果影响显著,氧化剂和...本文以辽河油田沈阳采油厂某采油作业区石油污染土壤为研究对象,探究H2O2浓度、FeSO4浓度、反应体系pH、水土比、反应时间等因素对石油污染土壤中石油烃降解效果的影响。研究结果表明,H2O2投加浓度对石油烃的降解效果影响显著,氧化剂和催化剂浓度对Fenton反应过程中石油烃的氧化效果有较大影响,反应体系pH值为6.0时石油烃的去除效果最佳,合理的水土比能够提高氧化效率。不同程度污染土壤的修复效果表明,反应24 h后,Fenton反应基本完成,石油烃去除率分别为49.22%,55.31%和61.98%,该研究结果可为污染土壤环境修复提供科学依据。In this paper, the effects of H2O2 concentration, FeSO4 concentration, reaction system pH, water and soil ratio, and reaction time on the degradation of petroleum hydrocarbons in oil-polluted soil were studied in an oil production area of Shenyang oil production plant of Liaohe Oilfield. The research results show that the concentration of H2O2 has a significant impact on the degradation effect of petroleum hydrocarbons, and the concentration of oxidant and catalyst has a great impact on the oxidation effect of petroleum hydrocarbons in the Fenton reaction process. When the pH value of the reaction system is 6.0, the removal effect of petroleum hydrocarbons is the best, and reasonable water and soil ratio can improve the oxidation efficiency. The remediation effects of contaminated soil of different degrees show that after 24 h of reaction, Fenton reaction is basically completed, and the removal rates of petroleum hydrocarbons are 49.22%, 55.31% and 61.98%, respectively. The research results can provide scientific basis for the remediation of contaminated soil environment.展开更多
To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absenc...To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absence of light instead of Fe(Ⅱ) and H 2O 2 was studied. Results showed that use of Fe (Ⅲ) is more promising than Fe(Ⅱ). The present study reflects that Fenton reaction is more efficient, in the presence of a small amount of salicylic acid is added which is a one of the priority pollutant.展开更多
This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficient...This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H_(2)O_(2)/HA/MF system, e.g., pH and the dosages of ZVI, HA and H_(2)O_(2), were investigated. Unlike the acid-favorable ZVI/H_(2)O_(2) and ZVI/H_(2)O_(2)/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. ^(·)OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H_(2)O_(2)/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(II) and local corrosion of iron. Large amounts of aqueous and bounded Fe(II) catalyzed H_(2)O_(2) to efficiently produce ^(·)OH, while HA maintained the surface and bulk cycles of Fe(II)/Fe(III). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.展开更多
Reactive oxygen species(ROSs)in Fenton process are of great importance in treating contaminants in wastewater.It is crucial to understand their chemical properties,formation,and reaction mechanisms with contaminants.T...Reactive oxygen species(ROSs)in Fenton process are of great importance in treating contaminants in wastewater.It is crucial to understand their chemical properties,formation,and reaction mechanisms with contaminants.This review summarizes the reactive oxygen species in Fenton process,including hydroxyl radical(·OH),superoxide radical(O_(2)·-),singlet oxygen(1O_(2)),hydroperoxyl radical(HO_(2)·),and high-valent iron.·OH shows a trend to react with chemistry groups with abundant electrons through H-atom abstraction,radical adduct formation and single electron transfer.Electron transfer is discovered to be an important pathway when1O_(2)degrades organic pollutants.Ring-opening andβ-scission are proposed to be the possible ways of1O_(2)to certain contaminants.Proton abstraction,nucleophilic substitution,and single electron transfer are proposed to explain how O_(2)·-degrade pollutants.As the conjugated acid of O_(2)·-,radical adduct formation and H-atom abstraction are reported for the reaction mechanisms of hydroperoxyl radical.High-valent iron in Fenton,namely Fe(IV),reacts with certain pollutants via single-or two-electron transfer.This review is important for researchers to understand the ROSs produced in Fenton and how they react with pollutants.展开更多
Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enha...Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enhancers for the removal of glycerin from saline water under ambient temperature by accelerating the ferric system.It was found that organics removal was not obviously affected by chloride ions of low concentration（less than 0.1 mol/L）,while the mineralization rate was strongly inhibited in the presence of a large amount of chloride ions.In addition,ferric hydrolysis-precipitation was significantly alleviated in the presence of HA and BQ,and HA was more effective in reducing ferric ions into ferrous ions than HA,while the H_2O_2 decomposition rate was higher in the BQ-Fenton system.Electron spin resonance analysis revealed that OH production was reduced in high salinity conditions,while it was enhanced after the addition of HA and BQ（especially HA）.This study provided a possible solution to control and alleviate the inhibitory effect of chloride ions on the Fenton process for organics removal.展开更多
The saline and buffered environment in actual wastewater imposes higher demands on Fenton and Fenton-like catalytic systems.This study developed a MoS_(2)co-catalytic Fe_(2)O_(3)Fenton-like system with controllable Le...The saline and buffered environment in actual wastewater imposes higher demands on Fenton and Fenton-like catalytic systems.This study developed a MoS_(2)co-catalytic Fe_(2)O_(3)Fenton-like system with controllable Lewis acid-base sites,achieving efficient treatment of various model pollutants and actual industrial wastewater under neutral buffered environment.The acidic microenvironment structured by the edge S sites(Lewis basic sites)in the MoS_(2)/Fe_(2)O_(3)catalyst is susceptible to the influence of Lewis acidic sites constructed by Mo and Fe element,affecting catalytic performance.Optimizing the ratio of precursor amounts ensures the stable presence of the acidic microenvironment on the surface of catalyst,enabling the beneficial co-catalytic effect of Mo sites to be realized.Furthermore,it transcends the rigid constraints imposed by the Fenton reaction on reaction environments,thereby expanding the applicability of commonplace oxides such as Fe_(2)O_(3)in actual industrial water remediation.展开更多
文摘The current modified electro-Fenton system was designed to develop a more convenient and efficient undivided system for practical wastewater treatment. The system adopted a cathode portion that employed magnetic stirring instead of common oxygen gas diffusion or gas sparging to supply oxygen gas for the electrolyte solution. Key factors influencing the cathode fabrication and activit） were investigated. The degradation of acid fuchsine with a self-made graphite-polytetrafluorethylene cathode was studied using spectrophotometer. It was found that the cathode generated hydrogen peroxide with high current efficiency and the hydrogen peroxide yield of the cathode did not decay after 10 times reuse. With the Pt anode at a ferrous ion concentration of 0.5 mmol/L, a pH of 3, and using magnetic stirring, dye decolorization could be rapidly accomplished but the destruction of benzene rings and intermediates was fairly difficult. With a Fe anode, dye degradation was more complete.
基金supported by the National Natural Science Foundation of China(41573118)Research Foundation of Education Bureau of Hunan Province,China(14B177)Special Project of Xiangtan University~~
文摘A novel plasmonic photo‐Fenton catalyst of Ag/AgCl/Fe‐S was synthesized by ion exchange and photoreduction methods.The obtained catalyst was characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,scanning electron microscope imaging,and Brunauer‐Emmett‐Teller measurements.Moreover,the photocatalytic activity of Ag/AgCl/Fe‐S was investigated for its degradation activity towards bisphenol A(BPA)as target pollutant under visible light irradiation.The effects of H2O2concentration,pH value,illumination intensity,and catalyst dosage on BPA degradation were examined.Our results indicated that the Ag/AgCl material was successfully loaded onto Fe‐sepiolite and showed a high photocatalytic activity under illumination by visible light.Furthermore,active species capture experiments were performed to explore the photocatalytic mechanism of the Ag/AgCl/Fe‐S in this heterogeneous photo‐Fenton process,where the major active species included hydroxyl radicals(?OH)and holes(h+).
基金supported by the National Natural Science Foundation of China(No.21906056No.22176060)+2 种基金the Undergraduate Training Program on Innovation and Entrepreneurship(S202110251087)the Science and Technology Commission of Shanghai Municipality(22ZR1418600)Shanghai Municipal Science and Technology(No.20DZ2250400).
文摘The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this problem.The original Fenton system relies on the hydroxyl radicals produced by Fe(Ⅱ)/H_(2)O_(2) to oxidize the organic contaminants.However,the application of the Fenton system is limited by its low iron cycling efficiency and the high risks of hydrogen peroxide transportation and storage.The introduction of external energy(including light and electricity etc.)can effectively promote the Fe(Ⅲ)/Fe(Ⅱ)cycle and the reduction of oxygen to produce hydrogen peroxide in situ.This review introduces three in-situ Fenton systems,which are electro-Fenton,Photo-Fenton,and chemical reaction.The mechanism,influencing factors,and catalysts of these three in-situ Fenton systems in degrading EOCs are discussed systematically.This review strengthens the understanding of Fenton and in-situ Fenton systems in degradation,offering further insight into the real application of the in-situ Fenton system in the removal of EOCs.
基金supported by the National Basic Research Program of China(No.2008CB417206)the National Natural Science Foundation of China(No.20877048)
文摘Under visible light illumination,2,3-diaminophenazine(DAPN)was generated from the oxidation of o-phenylenediamine(OPDA)in Fe^3+/H2O2 solution.Hydroxyl radical(*OH)produced in this system was determined by directly measuring the concentration of DAPN.In comparison with the traditional methods,the determination is more accurate and simple.
文摘本文以辽河油田沈阳采油厂某采油作业区石油污染土壤为研究对象,探究H2O2浓度、FeSO4浓度、反应体系pH、水土比、反应时间等因素对石油污染土壤中石油烃降解效果的影响。研究结果表明,H2O2投加浓度对石油烃的降解效果影响显著,氧化剂和催化剂浓度对Fenton反应过程中石油烃的氧化效果有较大影响,反应体系pH值为6.0时石油烃的去除效果最佳,合理的水土比能够提高氧化效率。不同程度污染土壤的修复效果表明,反应24 h后,Fenton反应基本完成,石油烃去除率分别为49.22%,55.31%和61.98%,该研究结果可为污染土壤环境修复提供科学依据。In this paper, the effects of H2O2 concentration, FeSO4 concentration, reaction system pH, water and soil ratio, and reaction time on the degradation of petroleum hydrocarbons in oil-polluted soil were studied in an oil production area of Shenyang oil production plant of Liaohe Oilfield. The research results show that the concentration of H2O2 has a significant impact on the degradation effect of petroleum hydrocarbons, and the concentration of oxidant and catalyst has a great impact on the oxidation effect of petroleum hydrocarbons in the Fenton reaction process. When the pH value of the reaction system is 6.0, the removal effect of petroleum hydrocarbons is the best, and reasonable water and soil ratio can improve the oxidation efficiency. The remediation effects of contaminated soil of different degrees show that after 24 h of reaction, Fenton reaction is basically completed, and the removal rates of petroleum hydrocarbons are 49.22%, 55.31% and 61.98%, respectively. The research results can provide scientific basis for the remediation of contaminated soil environment.
文摘To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absence of light instead of Fe(Ⅱ) and H 2O 2 was studied. Results showed that use of Fe (Ⅲ) is more promising than Fe(Ⅱ). The present study reflects that Fenton reaction is more efficient, in the presence of a small amount of salicylic acid is added which is a one of the priority pollutant.
基金supported by the National Natural Science Foundation of China (Nos. 21677055 and 22006045)the China Postdoctory Science Foundation (No. 2020M672361)the Project of Three Gorges Corporation (No. JD-ZC-FW-20-001)。
文摘This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H_(2)O_(2)/HA/MF system, e.g., pH and the dosages of ZVI, HA and H_(2)O_(2), were investigated. Unlike the acid-favorable ZVI/H_(2)O_(2) and ZVI/H_(2)O_(2)/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. ^(·)OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H_(2)O_(2)/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(II) and local corrosion of iron. Large amounts of aqueous and bounded Fe(II) catalyzed H_(2)O_(2) to efficiently produce ^(·)OH, while HA maintained the surface and bulk cycles of Fe(II)/Fe(III). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.
基金supported by the National Natural Science Foundation of China(Nos.22176102 and 21806081)Natural Science Foundation of Tianjin(No.19JCQNJC07900)+2 种基金Fundamental Research Funds for the Central UniversitiesNatural Science Foundation of Jiangsu Province in China(No.BK20230410)Natural Science Research of Jiangsu Higher Education Institution of China(No.23KJB610010)。
文摘Reactive oxygen species(ROSs)in Fenton process are of great importance in treating contaminants in wastewater.It is crucial to understand their chemical properties,formation,and reaction mechanisms with contaminants.This review summarizes the reactive oxygen species in Fenton process,including hydroxyl radical(·OH),superoxide radical(O_(2)·-),singlet oxygen(1O_(2)),hydroperoxyl radical(HO_(2)·),and high-valent iron.·OH shows a trend to react with chemistry groups with abundant electrons through H-atom abstraction,radical adduct formation and single electron transfer.Electron transfer is discovered to be an important pathway when1O_(2)degrades organic pollutants.Ring-opening andβ-scission are proposed to be the possible ways of1O_(2)to certain contaminants.Proton abstraction,nucleophilic substitution,and single electron transfer are proposed to explain how O_(2)·-degrade pollutants.As the conjugated acid of O_(2)·-,radical adduct formation and H-atom abstraction are reported for the reaction mechanisms of hydroperoxyl radical.High-valent iron in Fenton,namely Fe(IV),reacts with certain pollutants via single-or two-electron transfer.This review is important for researchers to understand the ROSs produced in Fenton and how they react with pollutants.
基金supported by the National Natural Science Foundation of China(Nos.51025830,41201498 and 51178360)
文摘Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enhancers for the removal of glycerin from saline water under ambient temperature by accelerating the ferric system.It was found that organics removal was not obviously affected by chloride ions of low concentration（less than 0.1 mol/L）,while the mineralization rate was strongly inhibited in the presence of a large amount of chloride ions.In addition,ferric hydrolysis-precipitation was significantly alleviated in the presence of HA and BQ,and HA was more effective in reducing ferric ions into ferrous ions than HA,while the H_2O_2 decomposition rate was higher in the BQ-Fenton system.Electron spin resonance analysis revealed that OH production was reduced in high salinity conditions,while it was enhanced after the addition of HA and BQ（especially HA）.This study provided a possible solution to control and alleviate the inhibitory effect of chloride ions on the Fenton process for organics removal.
基金supported by the National Natural Science Foundation of China(Nos.22176060 and 41876189)the Program of Shanghai Academic/Technology Research Leader(23XD1421000)+3 种基金Shanghai Municipal Science and Technology Major Project(Grant No.2018SHZDZX03)the Program of Introducing Talents of Discipline to Universities(B16017)Science and Technology Commission of Shanghai Municipality(20DZ2250400)the Fundamental Research Funds for the Central Universities(222201717003)。
文摘The saline and buffered environment in actual wastewater imposes higher demands on Fenton and Fenton-like catalytic systems.This study developed a MoS_(2)co-catalytic Fe_(2)O_(3)Fenton-like system with controllable Lewis acid-base sites,achieving efficient treatment of various model pollutants and actual industrial wastewater under neutral buffered environment.The acidic microenvironment structured by the edge S sites(Lewis basic sites)in the MoS_(2)/Fe_(2)O_(3)catalyst is susceptible to the influence of Lewis acidic sites constructed by Mo and Fe element,affecting catalytic performance.Optimizing the ratio of precursor amounts ensures the stable presence of the acidic microenvironment on the surface of catalyst,enabling the beneficial co-catalytic effect of Mo sites to be realized.Furthermore,it transcends the rigid constraints imposed by the Fenton reaction on reaction environments,thereby expanding the applicability of commonplace oxides such as Fe_(2)O_(3)in actual industrial water remediation.
