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
New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also du...New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also due to their adverse impacts on water ecological environment.Electro-Fenton technology is an effective method to remove PPCPs from water.Novel particle electrodes(MMT/rGO/Fe_(3)O_(4))were synthesized by depositing Fe3O4 nanoparticles on reduced graphene oxide modified montmorillonite and acted as catalysts to promote oxidation performance in a three-dimensional electro-Fenton(3D-EF)system.The electrodes combined the catalytic property of Fe3O4,hydrophilicity of montmorillonite and electrical conductivity of graphene oxides,and applied for the degradation of Acyclovir(ACV)with high efficiency and ease of operation.At optimal condition,the degradation rate of ACV reached 100%within 120 min,and the applicable pH range could be 3 to 11 in the 3D-EF system.The stability and reusability of MMT/rGO/Fe_(3)O_(4)particle electrodes were also studied,the removal rate of ACV remained at 92%after 10 cycles,which was just slightly lower than that of the first cycle.Potential degradation mechanisms were also proposed by methanol quenching tests and FT-ICR-MS.展开更多
Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic ...Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic catalyst selectivity,and electron transfer in O_(2)reduction remain major engineering obstacles.Here,we have proposed a systematic solution for efficient H_(2)O_(2)generation and its electro-Fenton(EF)application for refractory organic degradation based on the fabrication of a novel ZrO_(2)/CMK-3/PTFE cathode,in which polytetrafluoroethylene(PTFE)acted as a hydrophobic modifier to strengthen the O_(2)mass transfer,ZrO_(2)was adopted as a hydrophilic modifier to enhance the electron transfer of O_(2)reduction,and mesoporous carbon CMK-3 was utilized as a catalyst substrate to provide catalytic active sites.Moreover,feasible mass transfer of O_(2)from the hydrophobic to the hydrophilic layer was designed to increase the contact between O_(2)and the reaction interface.The H_(2)O_(2)yield of the ZrO_(2)/CMK-3/PTFE cathode was significantly improved by approximately 7.56 times compared to that of the co nventional gas diffusion cathode under the same conditions.The H_(2)O_(2)generation rate and Faraday efficiency reached125.98 mg·cm^(-2)·h^(-1)(normalized to 5674.04 mmol·g^(-1)·h^(-1)by catalyst loading)and 78.24%at-1.3 V versus standard hydrogen electrode(current density of-252 mA·cm^(-2)),respectively.The high H_(2)O_(2)yield ensured that sufficient OH was produced for excellent EF performance,resulting in a degradation efficiency of over 96%for refractory organics.This study offers a novel engineering solution for the efficient treatment of refractory wastewater using EF technology based on in situ high-yield H_(2)O_(2)electrosynthesis.展开更多
Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation...Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation efficiency was undertaken. It was found that Fenton process could not completely degrade citrate in the presence of hypophosphite since it caused a series inhibition. Therefore, UV light （photo-Fenton） or electron current （electro-Fenton） was applied to improve the degradation efficiency of the Fenton process. Results showed that both photo-Fenton and electro-Fenton processes could overcome the inhibition of hypophosphite, especially the electro-Fenton.展开更多
As a novel advanced oxidation process (AOP), electro-Fenton process is powerful for degrading most organic compounds including toxic and non-biodegradable ones, and so has attracted great attention. This paper reviews...As a novel advanced oxidation process (AOP), electro-Fenton process is powerful for degrading most organic compounds including toxic and non-biodegradable ones, and so has attracted great attention. This paper reviews this process in detail including the mechanism, electrolytic bath, electrode materials, aerations and operation parameters. The application of electro-Fenton method in wastewater treatment is evaluated and summarized. Future work in this field is suggested, and three main directions of new electrode exploitation, development of assisted technologies and mechanistic study should be strengthened.展开更多
This study reports the removal of amoxicillin(AMX)in aqueous media using the electroFenton process in the presence of a graphite cathode recovered from used batteries.The impact of the relevant parameters on the elect...This study reports the removal of amoxicillin(AMX)in aqueous media using the electroFenton process in the presence of a graphite cathode recovered from used batteries.The impact of the relevant parameters on the electroFenton process,namely the applied current intensity,the temperature,the initial concentration of AMX and the initial concentration of ferrous ions were investigated.The results showed that the optimal values were:I=600 mA,T=25℃,[AMX]_(0)=0.082 mmol·L^( 1) and[Fe^(2+)]=1 mmol·L^(1),leading to 95%degradation and 74%mineralization.The model parameters of AMX mineralization were determined using nonlinear methods,showing that it follows a pseudosecondorder kinetic.The Energy consumption(EC)calculated under the optimal values was found to be 0.79 kWhg 1,which was of the same order of magnitude of those reported in other findings;while it is noteworthy that the electrodes used in our study are of a lower cost.展开更多
The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degrada...The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degradation.Conventional Pd-catalytic EF process generates H_(2)O_(2) via the combination reaction of anodic O_(2) and cathodic H;.However,the relatively expensive catalyst limits its application.Herein,a hybrid Pd/activated carbon(Pd/AC)-stainless steel mesh(SS)cathode(PACSS)was proposed,which enables more efficie nt H_(2)O_(2)generation.It utilizes AC,the support of Pd catalyst,as part of cathode for H_(2)O_(2) generation via 2-electron anodic O_(2) reduction,and SS serve as a current distributor.Moreover,H_(2)O_(2) could be catalytically decomposed upon AC to generate highly reactive·OH,which avoids the use of Fe;.Compared with conventional Pd catalyst,H_(2)O_(2) concentration obtained by PACSS cathode is248.2%higher,the O_(2)utilization efficiency was also increased from 3.2%to 10.8%.Within 50 min,26.3%,72.5%,and 94.0%H_(2)O_(2) was decomposed by Pd,AC,and Pd/AC.Fluorescence detection results implied that Pd/AC is effective upon H_(2)O_(2) activation for·OH generation.Finally,iron-free EF process enabled by PACSS cathode was examined to be effective for reactive blue 19(RB19)degradation.After continuous running for 10 cycles(500 min),the PACSS cathode was still stable for H_(2)O_(2)generation,H_(2)O_(2)activation,and RB19 degradation,showing its potential application for organic pollutants degradation without increase in the running cost.展开更多
The flow-through electro-Fenton(EF-T)reactor with WBC cathode was designed to remove florfenicol(FF).The activated WBC cathode was prepared by facile carbonization and activation methods,and featured high specific sur...The flow-through electro-Fenton(EF-T)reactor with WBC cathode was designed to remove florfenicol(FF).The activated WBC cathode was prepared by facile carbonization and activation methods,and featured high specific surface area,natural multi-channel structure,abundant oxygen-containing groups,good hydrophilicity,and excellent O_(2)reducing capacity.WBC cathode was located above Ti/Ru-IrO_(2)mesh anode.O_(2)evolved at the anode was carried to the inner wall of channel of WBC by the force of buoyancy and water flow,which increases oxygen source of H_(2)O_(2)generation at the cathode.The flow-through system by using WBC electrode promote the mass transfer of O_(2)and FF.The production amount of H_(2)O_(2)at activated WBC was 32.2 mg/L,which was almost twice as much as that at non-activated WBC(15.0 mg/L).FF removal ratio in EF-T system was 98%,which was much higher than that of traditional flow-by electro-Fenton(EF-B,33%)or single electrooxidation system(EO,16%).EF-T system has the lowest energy consumption(4.367 kWh/kg)among the three electrochemical systems.The cathodic adsorption,anodic electrooxidation,and EF reaction are responsible for the degradation of FF.After five consecutive cycle experiments,FF removal ratio was still 98%,indicating WBC has the good stability.展开更多
Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficie...Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficient removal of organics.The simultaneous carbonization and ammonia etching of iron-based metal organic framework(Fe-MOF)materials yielded well-dispersed N-doped carbon-coated Fe_(3)N nanoparticles with a diameter of~70 nm.The Fe_(3)N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H_(2)O_(2) to•OH.The Fe_(3)N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching.A removal rate of 97-100%could be obtained for rhodamine B(RhB),dimethyl phthalate,methylene blue,and orange Ⅱ in 120 min at a pH of 5.0.When the solution pH was set to 3.0,5.0,7.0,and 9.0,the removal rate of RhB reached 100%,96%,92%,and 81%,respectively,in 60 min at an optimum voltage of 0.0 V(vs.reversible hydrogen electrode(RHE)).Moreover,the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0-9.0.In addition,the RhB removal efficiency remained as high as 90%after six cycles in the reusability experiments.This work highlights the MOF-derived Fe_(3)N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism,which facilitates its application in wastewater treatment.展开更多
A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-...A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al bifunctional catalyst could be separated from the solution directly and could synthesize H<sub>2</sub>O<sub>2</sub> in situ. The characterization results showed that Fe could improve the dispersion of Pd<sup>0</sup>, and the electronic interactions between Pd and Fe could increase the Pd<sup>0</sup> contents on the catalyst, which increased the productivity of H<sub>2</sub>O<sub>2</sub>. Furthermore, DFT calculations proved that the addition of Fe could inhibit the dissociation of O<sub>2</sub> and promote the nondissociative hydrogenation of O<sub>2</sub> on the surface of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al, which resulted in the increasement of H<sub>2</sub>O<sub>2</sub> selectivity. Finally, the in-situ synthesized H<sub>2</sub>O<sub>2</sub> by Pd was furtherly decomposed in situ by Fe to generate<span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span style="white-space:normal;color:#FFFFFF;font-family:Roboto, " background-color:#d46399;"=""><img src="Edit_e6a13073-7151-40b7-b2c3-a59a59d064fc.png" alt="" /></span></span></span>OH radicals to degrade organic pollutants. Therefore, Fe-Pd/ γ-Al<sub>2</sub>O<sub>3</sub>/Al catalysts exhibited excellent catalytic activity in the in-situ synthesis of H<sub>2</sub>O<sub>2</sub> and the degradation of RhB due to the synergistic effects between Pd and Fe on the catalyst. It provided a new idea for the design of bifunctional electro-Fenton catalysts. Ten cycles of experiments showed that the catalytic activity of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al catalyst could be maintained for a long time.展开更多
The Electrochemical advanced oxidation method “Electro-Fenton” has been applied to remove 17β-estradiol (17β)- estra-1,3,5(10)-triéne-3,17-diol) in aqueous-acetonitrile mixture. This endocrine disrupting is a...The Electrochemical advanced oxidation method “Electro-Fenton” has been applied to remove 17β-estradiol (17β)- estra-1,3,5(10)-triéne-3,17-diol) in aqueous-acetonitrile mixture. This endocrine disrupting is a steroid hormone, releases from humans, animals and residual pharmaceuticals into the environmental water and usually causes suspected undesirable effects in aquatic organisms. The degradation of this organic compound by Electro-Fenton process was showed using a carbon felt cathode and platinum anode. The evolution of the concentration during treatment was followed up by high performance liquid chromatography (HPLC). The influence of operating conditions on the degradation of 17β-estradiol by Electro-Fenton step, such as initial concentration and catalyst concentration, has been investi- gated and discussed. We showed that the degradation reaction obeyed apparent first-order reaction kinetics, with absolute rate constant determined as 5.12 × 109 M–1 s–1 by competitive kinetics method taking Benzoic Acid as reference compound. The results confirm the efficiency of the Electro-Fenton process to degrade organic pollutant in aqueous-acetonitrile mixture.展开更多
Membrane distillation(MD)is a promising alternative desalination technology,but the hydrophobic membrane cannot intercept volatile organic compounds(VOCs),resulting in aggravation in the quality of permeate.In term of...Membrane distillation(MD)is a promising alternative desalination technology,but the hydrophobic membrane cannot intercept volatile organic compounds(VOCs),resulting in aggravation in the quality of permeate.In term of this,electro-Fenton(EF)was coupled with sweeping gas membrane distillation(SGMD)in a more efficient way to construct an advanced oxidation barrier at the gas-liquid interface,so that the VOCs could be trapped in this layer to guarantee the water quality of the distillate.During the so-called EF-MD process,an interfacial interception barrier containing hydroxyl radical formed on the hydrophobic membrane surface.It contributed to the high phenol rejection of 90.2% with the permeate phenol concentration lower than 1.50 mg/L.Effective interceptions can be achieved in a wide temperature range,even though the permeate flux of phenol was also intensified.The EF-MD system was robust to high salinity and could electrochemically regenerate ferrous ions,which endowed the long-term stability of the system.This novel EF-MD configuration proposed a valuable strategy to intercept VOCs in MD and will broaden the application of MD in hypersaline wastewater treatment.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the GDAS’Project of Science and Technology Development(No.2020GDASYL-20200103044)Key-Area Research and Development Program of Guangdong(No.2020B1111350002)+1 种基金the National Key R&D Program of China(No.2019YFC1805305)the Project of Water Resource Department of Guangdong Province(No.2017-18).
文摘New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also due to their adverse impacts on water ecological environment.Electro-Fenton technology is an effective method to remove PPCPs from water.Novel particle electrodes(MMT/rGO/Fe_(3)O_(4))were synthesized by depositing Fe3O4 nanoparticles on reduced graphene oxide modified montmorillonite and acted as catalysts to promote oxidation performance in a three-dimensional electro-Fenton(3D-EF)system.The electrodes combined the catalytic property of Fe3O4,hydrophilicity of montmorillonite and electrical conductivity of graphene oxides,and applied for the degradation of Acyclovir(ACV)with high efficiency and ease of operation.At optimal condition,the degradation rate of ACV reached 100%within 120 min,and the applicable pH range could be 3 to 11 in the 3D-EF system.The stability and reusability of MMT/rGO/Fe_(3)O_(4)particle electrodes were also studied,the removal rate of ACV remained at 92%after 10 cycles,which was just slightly lower than that of the first cycle.Potential degradation mechanisms were also proposed by methanol quenching tests and FT-ICR-MS.
基金National Natural Science Foundation of China(22176125,52200103 and22178220)China Postdoctoral Science Foundation(2022 M722081 and 2021 M692064)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Center for Advanced Electronic Materials and Devices and the instrumental Analysis Center,School of Environmental Science and Engineering,Shanghai Jiao Tong University for support。
文摘Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic catalyst selectivity,and electron transfer in O_(2)reduction remain major engineering obstacles.Here,we have proposed a systematic solution for efficient H_(2)O_(2)generation and its electro-Fenton(EF)application for refractory organic degradation based on the fabrication of a novel ZrO_(2)/CMK-3/PTFE cathode,in which polytetrafluoroethylene(PTFE)acted as a hydrophobic modifier to strengthen the O_(2)mass transfer,ZrO_(2)was adopted as a hydrophilic modifier to enhance the electron transfer of O_(2)reduction,and mesoporous carbon CMK-3 was utilized as a catalyst substrate to provide catalytic active sites.Moreover,feasible mass transfer of O_(2)from the hydrophobic to the hydrophilic layer was designed to increase the contact between O_(2)and the reaction interface.The H_(2)O_(2)yield of the ZrO_(2)/CMK-3/PTFE cathode was significantly improved by approximately 7.56 times compared to that of the co nventional gas diffusion cathode under the same conditions.The H_(2)O_(2)generation rate and Faraday efficiency reached125.98 mg·cm^(-2)·h^(-1)(normalized to 5674.04 mmol·g^(-1)·h^(-1)by catalyst loading)and 78.24%at-1.3 V versus standard hydrogen electrode(current density of-252 mA·cm^(-2)),respectively.The high H_(2)O_(2)yield ensured that sufficient OH was produced for excellent EF performance,resulting in a degradation efficiency of over 96%for refractory organics.This study offers a novel engineering solution for the efficient treatment of refractory wastewater using EF technology based on in situ high-yield H_(2)O_(2)electrosynthesis.
基金The authors thank the "National" Science Council, Taiwan, China for financially supporting (No. NSC95- 2211-E-006-032).
文摘Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation efficiency was undertaken. It was found that Fenton process could not completely degrade citrate in the presence of hypophosphite since it caused a series inhibition. Therefore, UV light （photo-Fenton） or electron current （electro-Fenton） was applied to improve the degradation efficiency of the Fenton process. Results showed that both photo-Fenton and electro-Fenton processes could overcome the inhibition of hypophosphite, especially the electro-Fenton.
基金Project supported by the National Natural Science Foundation of China (No. 50478049)the Natural Science Foundation of Guangdong Province (No. 04011215), China
文摘As a novel advanced oxidation process (AOP), electro-Fenton process is powerful for degrading most organic compounds including toxic and non-biodegradable ones, and so has attracted great attention. This paper reviews this process in detail including the mechanism, electrolytic bath, electrode materials, aerations and operation parameters. The application of electro-Fenton method in wastewater treatment is evaluated and summarized. Future work in this field is suggested, and three main directions of new electrode exploitation, development of assisted technologies and mechanistic study should be strengthened.
文摘This study reports the removal of amoxicillin(AMX)in aqueous media using the electroFenton process in the presence of a graphite cathode recovered from used batteries.The impact of the relevant parameters on the electroFenton process,namely the applied current intensity,the temperature,the initial concentration of AMX and the initial concentration of ferrous ions were investigated.The results showed that the optimal values were:I=600 mA,T=25℃,[AMX]_(0)=0.082 mmol·L^( 1) and[Fe^(2+)]=1 mmol·L^(1),leading to 95%degradation and 74%mineralization.The model parameters of AMX mineralization were determined using nonlinear methods,showing that it follows a pseudosecondorder kinetic.The Energy consumption(EC)calculated under the optimal values was found to be 0.79 kWhg 1,which was of the same order of magnitude of those reported in other findings;while it is noteworthy that the electrodes used in our study are of a lower cost.
基金financially supported by the National Natural Science Foundation of China(Nos.52006049,51776055)the China Postdoctoral Science Foundation(Nos.2019M661293,2020T130149)。
文摘The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degradation.Conventional Pd-catalytic EF process generates H_(2)O_(2) via the combination reaction of anodic O_(2) and cathodic H;.However,the relatively expensive catalyst limits its application.Herein,a hybrid Pd/activated carbon(Pd/AC)-stainless steel mesh(SS)cathode(PACSS)was proposed,which enables more efficie nt H_(2)O_(2)generation.It utilizes AC,the support of Pd catalyst,as part of cathode for H_(2)O_(2) generation via 2-electron anodic O_(2) reduction,and SS serve as a current distributor.Moreover,H_(2)O_(2) could be catalytically decomposed upon AC to generate highly reactive·OH,which avoids the use of Fe;.Compared with conventional Pd catalyst,H_(2)O_(2) concentration obtained by PACSS cathode is248.2%higher,the O_(2)utilization efficiency was also increased from 3.2%to 10.8%.Within 50 min,26.3%,72.5%,and 94.0%H_(2)O_(2) was decomposed by Pd,AC,and Pd/AC.Fluorescence detection results implied that Pd/AC is effective upon H_(2)O_(2) activation for·OH generation.Finally,iron-free EF process enabled by PACSS cathode was examined to be effective for reactive blue 19(RB19)degradation.After continuous running for 10 cycles(500 min),the PACSS cathode was still stable for H_(2)O_(2)generation,H_(2)O_(2)activation,and RB19 degradation,showing its potential application for organic pollutants degradation without increase in the running cost.
基金supported by the National Science Fund for Distinguished Young Scholars(No.51625801)Major Science and Technology Program for Water Pollution Control and Treatment in China(No.2017ZX07202-001-007)+4 种基金Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme(2017)Guangdong Provincial Science and Technology Project(No.2017A020216014)the National Natural Science Foundation of China(No.21777106)Pearl River S&T Nova Program of Guangzhou,China(No.201710010065)Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology(No.2020B1212060022)。
文摘The flow-through electro-Fenton(EF-T)reactor with WBC cathode was designed to remove florfenicol(FF).The activated WBC cathode was prepared by facile carbonization and activation methods,and featured high specific surface area,natural multi-channel structure,abundant oxygen-containing groups,good hydrophilicity,and excellent O_(2)reducing capacity.WBC cathode was located above Ti/Ru-IrO_(2)mesh anode.O_(2)evolved at the anode was carried to the inner wall of channel of WBC by the force of buoyancy and water flow,which increases oxygen source of H_(2)O_(2)generation at the cathode.The flow-through system by using WBC electrode promote the mass transfer of O_(2)and FF.The production amount of H_(2)O_(2)at activated WBC was 32.2 mg/L,which was almost twice as much as that at non-activated WBC(15.0 mg/L).FF removal ratio in EF-T system was 98%,which was much higher than that of traditional flow-by electro-Fenton(EF-B,33%)or single electrooxidation system(EO,16%).EF-T system has the lowest energy consumption(4.367 kWh/kg)among the three electrochemical systems.The cathodic adsorption,anodic electrooxidation,and EF reaction are responsible for the degradation of FF.After five consecutive cycle experiments,FF removal ratio was still 98%,indicating WBC has the good stability.
文摘Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficient removal of organics.The simultaneous carbonization and ammonia etching of iron-based metal organic framework(Fe-MOF)materials yielded well-dispersed N-doped carbon-coated Fe_(3)N nanoparticles with a diameter of~70 nm.The Fe_(3)N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H_(2)O_(2) to•OH.The Fe_(3)N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching.A removal rate of 97-100%could be obtained for rhodamine B(RhB),dimethyl phthalate,methylene blue,and orange Ⅱ in 120 min at a pH of 5.0.When the solution pH was set to 3.0,5.0,7.0,and 9.0,the removal rate of RhB reached 100%,96%,92%,and 81%,respectively,in 60 min at an optimum voltage of 0.0 V(vs.reversible hydrogen electrode(RHE)).Moreover,the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0-9.0.In addition,the RhB removal efficiency remained as high as 90%after six cycles in the reusability experiments.This work highlights the MOF-derived Fe_(3)N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism,which facilitates its application in wastewater treatment.
文摘A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al bifunctional catalyst could be separated from the solution directly and could synthesize H<sub>2</sub>O<sub>2</sub> in situ. The characterization results showed that Fe could improve the dispersion of Pd<sup>0</sup>, and the electronic interactions between Pd and Fe could increase the Pd<sup>0</sup> contents on the catalyst, which increased the productivity of H<sub>2</sub>O<sub>2</sub>. Furthermore, DFT calculations proved that the addition of Fe could inhibit the dissociation of O<sub>2</sub> and promote the nondissociative hydrogenation of O<sub>2</sub> on the surface of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al, which resulted in the increasement of H<sub>2</sub>O<sub>2</sub> selectivity. Finally, the in-situ synthesized H<sub>2</sub>O<sub>2</sub> by Pd was furtherly decomposed in situ by Fe to generate<span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span style="white-space:normal;color:#FFFFFF;font-family:Roboto, " background-color:#d46399;"=""><img src="Edit_e6a13073-7151-40b7-b2c3-a59a59d064fc.png" alt="" /></span></span></span>OH radicals to degrade organic pollutants. Therefore, Fe-Pd/ γ-Al<sub>2</sub>O<sub>3</sub>/Al catalysts exhibited excellent catalytic activity in the in-situ synthesis of H<sub>2</sub>O<sub>2</sub> and the degradation of RhB due to the synergistic effects between Pd and Fe on the catalyst. It provided a new idea for the design of bifunctional electro-Fenton catalysts. Ten cycles of experiments showed that the catalytic activity of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al catalyst could be maintained for a long time.
文摘The Electrochemical advanced oxidation method “Electro-Fenton” has been applied to remove 17β-estradiol (17β)- estra-1,3,5(10)-triéne-3,17-diol) in aqueous-acetonitrile mixture. This endocrine disrupting is a steroid hormone, releases from humans, animals and residual pharmaceuticals into the environmental water and usually causes suspected undesirable effects in aquatic organisms. The degradation of this organic compound by Electro-Fenton process was showed using a carbon felt cathode and platinum anode. The evolution of the concentration during treatment was followed up by high performance liquid chromatography (HPLC). The influence of operating conditions on the degradation of 17β-estradiol by Electro-Fenton step, such as initial concentration and catalyst concentration, has been investi- gated and discussed. We showed that the degradation reaction obeyed apparent first-order reaction kinetics, with absolute rate constant determined as 5.12 × 109 M–1 s–1 by competitive kinetics method taking Benzoic Acid as reference compound. The results confirm the efficiency of the Electro-Fenton process to degrade organic pollutant in aqueous-acetonitrile mixture.
基金supported by the National Natural Science Foundation of China(Nos.52200111,51978651,and 51878049)the China Postdoctoral Science Foundation(No.2021M703407)the special fund from the State Key Joint Laboratory of Environment Simulation and Pollution Control(Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences(No.21Z01ESPCR)。
文摘Membrane distillation(MD)is a promising alternative desalination technology,but the hydrophobic membrane cannot intercept volatile organic compounds(VOCs),resulting in aggravation in the quality of permeate.In term of this,electro-Fenton(EF)was coupled with sweeping gas membrane distillation(SGMD)in a more efficient way to construct an advanced oxidation barrier at the gas-liquid interface,so that the VOCs could be trapped in this layer to guarantee the water quality of the distillate.During the so-called EF-MD process,an interfacial interception barrier containing hydroxyl radical formed on the hydrophobic membrane surface.It contributed to the high phenol rejection of 90.2% with the permeate phenol concentration lower than 1.50 mg/L.Effective interceptions can be achieved in a wide temperature range,even though the permeate flux of phenol was also intensified.The EF-MD system was robust to high salinity and could electrochemically regenerate ferrous ions,which endowed the long-term stability of the system.This novel EF-MD configuration proposed a valuable strategy to intercept VOCs in MD and will broaden the application of MD in hypersaline wastewater treatment.
