Advanced processes for peroxymonosulfate(PMS)-based oxidation are efficient in eliminating toxic and refractory organic pol-lutants from sewage.The activation of electron-withdrawing HSO_(5)^(-)releases reactive speci...Advanced processes for peroxymonosulfate(PMS)-based oxidation are efficient in eliminating toxic and refractory organic pol-lutants from sewage.The activation of electron-withdrawing HSO_(5)^(-)releases reactive species,including sulfate radical(·SO_(4)^(-)),hydroxyl radical(·OH),superoxide radical(·O_(2)^(-)),and singlet oxygen(1O_(2)),which can induce the degradation of organic contaminants.In this work,we synthesized a variety of M-OMS-2 nanorods(M=Co,Ni,Cu,Fe)by doping Co^(2+),Ni^(2+),Cu^(2+),or Fe^(3+)into manganese oxide oc-tahedral molecular sieve(OMS-2)to efficiently remove sulfamethoxazole(SMX)via PMS activation.The catalytic performance of M-OMS-2 in SMX elimination via PMS activation was assessed.The nanorods obtained in decreasing order of SMX removal rate were Cu-OMS-2(96.40%),Co-OMS-2(88.00%),Ni-OMS-2(87.20%),Fe-OMS-2(35.00%),and OMS-2(33.50%).Then,the kinetics and struc-ture-activity relationship of the M-OMS-2 nanorods during the elimination of SMX were investigated.The feasible mechanism underly-ing SMX degradation by the Cu-OMS-2/PMS system was further investigated with a quenching experiment,high-resolution mass spec-troscopy,and electron paramagnetic resonance.Results showed that SMX degradation efficiency was enhanced in seawater and tap water,demonstrating the potential application of Cu-OMS-2/PMS system in sewage treatment.展开更多
The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,th...The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.展开更多
As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemmin...As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.展开更多
This work uses thermal polymerization of urea nitrate,oxyacetic acid and urea as the raw material to prepare ultra-thin porous carbon nitride with carbon defects and C-O band(OA-UN-CN).Density functional theory(DFT)ca...This work uses thermal polymerization of urea nitrate,oxyacetic acid and urea as the raw material to prepare ultra-thin porous carbon nitride with carbon defects and C-O band(OA-UN-CN).Density functional theory(DFT)calculations showed OA-UN-CN had narrower band gap,faster electron transport and a new internal construction electric field.Additionally,the prepared OA-UN-CN significantly enhanced photocatalytic activation of peroxymonosulfate(PMS)due to enhanced light absorption performance and faster electron overflow.As the result,the OA-UN-CN/PMS could entirely degrade bisphenol A(BPA)within 30 min,where the photodegradation rate was 81.8 and 7.9 times higher than that of g-C_(3)N_(4)and OA-UN-CN,respectively.Beyond,the OA-UN-CN/PMS could likewise degrade other bisphenol pollutants and sodium lignosulfonate efficiently.We suggested possible photocatalytic degradation pathways accordingly and explored the toxicity of its degradation products.This work provides a new idea on the development of advanced photocatalytic oxidation processes for the treatment of bisphenol pollutants and lignin derivatives,via a metal-free photothermal-catalyst.展开更多
With the continuous deepening of rural revitalization strategy and the increasingly strict sewage discharge standards,rural domestic sewage treatment technology is facing higher challenges and requirements.The combine...With the continuous deepening of rural revitalization strategy and the increasingly strict sewage discharge standards,rural domestic sewage treatment technology is facing higher challenges and requirements.The combined process of micro-electrolysis+micro-nano bubbles coupled with peroxymonosulfate was constructed in this study,and the treatment effect and application value of this technology were explored with the actual rural domestic sewage as the treatment object.The experimental results showed that under the conditions of HRT of 120 min,PMS dosage of 0.15 mmol/L,pH=7,MBs air intake of 15 ml/min,current intensity of 15 A,and Fe/C mass ratio of 1:1,the removal rates of COD,ammonia nitrogen and total phosphorus can reach 88.55%,77.18%and 74.67%,respectively.Under the condition that the pH value of sewage was not adjusted,the non-biochemical simultaneous decarbonization,denitrification and phosphorus removal of rural domestic sewage can be achieved by micro-electrolysis and micro-nano bubbles coupled with peroxymonosulfate.The concentrations of effluent COD,ammonia nitrogen and total phosphorus met the requirements of the first level standard of the Discharge Standard of Water Pollutants for Rural Domestic Sewage Treatment Facilities(DB45T2413-2021).And the comprehensive operating cost was about 1.15 yuan/m 3.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21972073,22136003,22206188,and 21805166).
文摘Advanced processes for peroxymonosulfate(PMS)-based oxidation are efficient in eliminating toxic and refractory organic pol-lutants from sewage.The activation of electron-withdrawing HSO_(5)^(-)releases reactive species,including sulfate radical(·SO_(4)^(-)),hydroxyl radical(·OH),superoxide radical(·O_(2)^(-)),and singlet oxygen(1O_(2)),which can induce the degradation of organic contaminants.In this work,we synthesized a variety of M-OMS-2 nanorods(M=Co,Ni,Cu,Fe)by doping Co^(2+),Ni^(2+),Cu^(2+),or Fe^(3+)into manganese oxide oc-tahedral molecular sieve(OMS-2)to efficiently remove sulfamethoxazole(SMX)via PMS activation.The catalytic performance of M-OMS-2 in SMX elimination via PMS activation was assessed.The nanorods obtained in decreasing order of SMX removal rate were Cu-OMS-2(96.40%),Co-OMS-2(88.00%),Ni-OMS-2(87.20%),Fe-OMS-2(35.00%),and OMS-2(33.50%).Then,the kinetics and struc-ture-activity relationship of the M-OMS-2 nanorods during the elimination of SMX were investigated.The feasible mechanism underly-ing SMX degradation by the Cu-OMS-2/PMS system was further investigated with a quenching experiment,high-resolution mass spec-troscopy,and electron paramagnetic resonance.Results showed that SMX degradation efficiency was enhanced in seawater and tap water,demonstrating the potential application of Cu-OMS-2/PMS system in sewage treatment.
基金gratefully acknowledge the financial support of the National Natural Science Foundation of China(22108145 and 21978143)the Shandong Province Natural Science Foundation(ZR2020QB189)+1 种基金State Key Laboratory of Heavy Oil Processing(SKLHOP202203008)the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2201).
文摘The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.
基金funded by the Natural Science Foundation of Fujian Province(2023J05180)the President's Foundation of Minnan Normal University(KJ2021011).
文摘As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.
基金the National Natural Science Foundation of China(No.22076068,8111310014)(China)the University of Calgary’s Canada First Research Excellence Fund(CFREF)program(Canada)for financial support。
文摘This work uses thermal polymerization of urea nitrate,oxyacetic acid and urea as the raw material to prepare ultra-thin porous carbon nitride with carbon defects and C-O band(OA-UN-CN).Density functional theory(DFT)calculations showed OA-UN-CN had narrower band gap,faster electron transport and a new internal construction electric field.Additionally,the prepared OA-UN-CN significantly enhanced photocatalytic activation of peroxymonosulfate(PMS)due to enhanced light absorption performance and faster electron overflow.As the result,the OA-UN-CN/PMS could entirely degrade bisphenol A(BPA)within 30 min,where the photodegradation rate was 81.8 and 7.9 times higher than that of g-C_(3)N_(4)and OA-UN-CN,respectively.Beyond,the OA-UN-CN/PMS could likewise degrade other bisphenol pollutants and sodium lignosulfonate efficiently.We suggested possible photocatalytic degradation pathways accordingly and explored the toxicity of its degradation products.This work provides a new idea on the development of advanced photocatalytic oxidation processes for the treatment of bisphenol pollutants and lignin derivatives,via a metal-free photothermal-catalyst.
基金Supported by Research Foundation Ability Enhancement Project for Young and Middle-aged Teachers in Guangxi Universities(2023KY2049).
文摘With the continuous deepening of rural revitalization strategy and the increasingly strict sewage discharge standards,rural domestic sewage treatment technology is facing higher challenges and requirements.The combined process of micro-electrolysis+micro-nano bubbles coupled with peroxymonosulfate was constructed in this study,and the treatment effect and application value of this technology were explored with the actual rural domestic sewage as the treatment object.The experimental results showed that under the conditions of HRT of 120 min,PMS dosage of 0.15 mmol/L,pH=7,MBs air intake of 15 ml/min,current intensity of 15 A,and Fe/C mass ratio of 1:1,the removal rates of COD,ammonia nitrogen and total phosphorus can reach 88.55%,77.18%and 74.67%,respectively.Under the condition that the pH value of sewage was not adjusted,the non-biochemical simultaneous decarbonization,denitrification and phosphorus removal of rural domestic sewage can be achieved by micro-electrolysis and micro-nano bubbles coupled with peroxymonosulfate.The concentrations of effluent COD,ammonia nitrogen and total phosphorus met the requirements of the first level standard of the Discharge Standard of Water Pollutants for Rural Domestic Sewage Treatment Facilities(DB45T2413-2021).And the comprehensive operating cost was about 1.15 yuan/m 3.
