Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-c...Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect,giving rise to the sluggish Fe^(2+)/Fe^(3+)cycle and low dynamic concentration of Fe^(2+)for ROS production.Herein,we present a three-dimensional(3D)macroscale co-catalyst functionalized with molybdenum disulfide(MoS_(2))to achieve ultra-efficient Fe^(2+)regeneration(equilibrium Fe^(2+)ratio of 82.4%)and remarkable stability(more than 20 cycles)via a circulating flow-through process.Unlike the conventional batch-type reactor,experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode,initiated by the convectionenhanced mass/charge transfer for Fe^(2+)reduction and then strengthened by MoS_(2)-induced flow rotation for sufficient reactant mixing,is crucial for oxidant activation and subsequent ROS generation.Strikingly,the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency.Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology,especially in large-scale complex wastewater treatment.展开更多
Nano-Fe2O3/goldmine complex was obtained by chemical coprecipitation reaction on the surface of goldmine waste-solid. Being used as the heterogeneous catalyst in Fenton-like advanced oxidation processes (AOPs), its tr...Nano-Fe2O3/goldmine complex was obtained by chemical coprecipitation reaction on the surface of goldmine waste-solid. Being used as the heterogeneous catalyst in Fenton-like advanced oxidation processes (AOPs), its treatment effect was studied in the removal performance of industrial dyes effluent. Although the maximal COD removal efficiency would reach 35.4% when 5 mL NaClO was added in 100 mL industrial dyes effluent, it is found that by using nano-Fe2O3/goldmine system, the COD removal efficiency of 13,000 mg/L dyes wastewater could reach up to 75.5% in the presence of 30 g/L nano-Fe2O3/goldmine complex and 50 mL/L NaClO at 50。C.展开更多
Triallyl isocyanurate(TAIC,C12H15N3O3)has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact.TAIC degradation was enhanced ...Triallyl isocyanurate(TAIC,C12H15N3O3)has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact.TAIC degradation was enhanced when an ozone(O3)/ultraviolet(UV)process was applied compared with the application of an independent O3 process.Although 99%of TAIC could be degraded in 5 min during both processes,the O3/UV process had a 70%mineralization rate that was much higher than that of the independent O3 process(9%)in 30 min.Four possible degradation pathways were proposed based on the organic compounds of intermediate products identified during TAIC degradation through the application of independent 03 and O3/UV processes.pH impacted both the direct and indirect oxidation processes.Acidic and alkaline conditions preferred direct and indirect reactions respectively,with a pH of 9 achieving maximum Total Organic Carbon(TOC)removal.Both CO32-and HCO3-decreased TOC removal,however only CO32-negatively impacted TAIC degradation.Effects of Cl-as a radical scavenger became more marked only at high concentrations(over 500 mg/L Cl-).Particulate and suspended matter could hinder the transmission of ultraviolet light and reduce the production of HO·accordingly.展开更多
Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH r...Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range.Herein,we fabricate surface Co defect-rich spinel ZnCo_(2)O_(4)porous nanosheets,which can generate≡CoIV=O and ^(1)O_(2) over a wide pH range of 3.81-10.96 by the formation of amphoteric≡Zn(OH)2 in peroxymonosulfate(PMS)activation process.Density functional theory(DFT)calculations show Co defect-rich ZnCo_(2)O_(4)possesses much stronger adsorption ability and more electron transfer to PMS.Moreover,the adsorption mode changes from terminal oxygen Co-O-Co to Co-O,accelerating the polarization of adjacent oxygen,which is beneficial to the generation of≡CoIV=O and Generating ^(1)O_(2) .Co defect-rich ZnCo_(2)O_(4)porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol(PNP)degradation,whose toxicity of degradation intermediates is significant reduction.The Co defect-rich ZnCo_(2)O_(4)nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93%over 10 h.This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.展开更多
基金supported by National Natural Science Foundation of China(52003240)Zhejiang Provincial Natural Science Foundation of China(LQ21B070007)China Postdoctoral Science Foundation(2022M722818).
文摘Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect,giving rise to the sluggish Fe^(2+)/Fe^(3+)cycle and low dynamic concentration of Fe^(2+)for ROS production.Herein,we present a three-dimensional(3D)macroscale co-catalyst functionalized with molybdenum disulfide(MoS_(2))to achieve ultra-efficient Fe^(2+)regeneration(equilibrium Fe^(2+)ratio of 82.4%)and remarkable stability(more than 20 cycles)via a circulating flow-through process.Unlike the conventional batch-type reactor,experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode,initiated by the convectionenhanced mass/charge transfer for Fe^(2+)reduction and then strengthened by MoS_(2)-induced flow rotation for sufficient reactant mixing,is crucial for oxidant activation and subsequent ROS generation.Strikingly,the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency.Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology,especially in large-scale complex wastewater treatment.
文摘Nano-Fe2O3/goldmine complex was obtained by chemical coprecipitation reaction on the surface of goldmine waste-solid. Being used as the heterogeneous catalyst in Fenton-like advanced oxidation processes (AOPs), its treatment effect was studied in the removal performance of industrial dyes effluent. Although the maximal COD removal efficiency would reach 35.4% when 5 mL NaClO was added in 100 mL industrial dyes effluent, it is found that by using nano-Fe2O3/goldmine system, the COD removal efficiency of 13,000 mg/L dyes wastewater could reach up to 75.5% in the presence of 30 g/L nano-Fe2O3/goldmine complex and 50 mL/L NaClO at 50。C.
基金This work was supported by the Major Science and Technology Program for Water Pollution Control and Treatment of China(Nos.2018ZX07105004 and 2018ZX07105003).
文摘Triallyl isocyanurate(TAIC,C12H15N3O3)has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact.TAIC degradation was enhanced when an ozone(O3)/ultraviolet(UV)process was applied compared with the application of an independent O3 process.Although 99%of TAIC could be degraded in 5 min during both processes,the O3/UV process had a 70%mineralization rate that was much higher than that of the independent O3 process(9%)in 30 min.Four possible degradation pathways were proposed based on the organic compounds of intermediate products identified during TAIC degradation through the application of independent 03 and O3/UV processes.pH impacted both the direct and indirect oxidation processes.Acidic and alkaline conditions preferred direct and indirect reactions respectively,with a pH of 9 achieving maximum Total Organic Carbon(TOC)removal.Both CO32-and HCO3-decreased TOC removal,however only CO32-negatively impacted TAIC degradation.Effects of Cl-as a radical scavenger became more marked only at high concentrations(over 500 mg/L Cl-).Particulate and suspended matter could hinder the transmission of ultraviolet light and reduce the production of HO·accordingly.
基金supported by the National Natural Science Foundation of China(NSFC)(No.22308336).
文摘Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range.Herein,we fabricate surface Co defect-rich spinel ZnCo_(2)O_(4)porous nanosheets,which can generate≡CoIV=O and ^(1)O_(2) over a wide pH range of 3.81-10.96 by the formation of amphoteric≡Zn(OH)2 in peroxymonosulfate(PMS)activation process.Density functional theory(DFT)calculations show Co defect-rich ZnCo_(2)O_(4)possesses much stronger adsorption ability and more electron transfer to PMS.Moreover,the adsorption mode changes from terminal oxygen Co-O-Co to Co-O,accelerating the polarization of adjacent oxygen,which is beneficial to the generation of≡CoIV=O and Generating ^(1)O_(2) .Co defect-rich ZnCo_(2)O_(4)porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol(PNP)degradation,whose toxicity of degradation intermediates is significant reduction.The Co defect-rich ZnCo_(2)O_(4)nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93%over 10 h.This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.
