Organic micropollutants,with high toxicity and environmental concern,are present in the landfill leachate at much lower levels than total organic constituents (chemical oxygen demand (COD),biochemical oxygen demand (B...Organic micropollutants,with high toxicity and environmental concern,are present in the landfill leachate at much lower levels than total organic constituents (chemical oxygen demand (COD),biochemical oxygen demand (BOD),or total organic carbon (TOC)),and few has been known for their behaviors in different treatment processes.In this study,occurrence and removal of 17 organochlorine pesticides (OCPs),16 polycyclic aromatic hydrocarbons (PAHs),and technical 4-nonylphenol (4-NP) in landfill leachate in a comb...展开更多
Activated carbon is employed for the adsorption of organic micropollutants(OMPs)from water,typically present in concentrations ranging from ng L1 to mg L1.However,the efficacy of OMP removal is considerably deteriorat...Activated carbon is employed for the adsorption of organic micropollutants(OMPs)from water,typically present in concentrations ranging from ng L1 to mg L1.However,the efficacy of OMP removal is considerably deteriorated due to competitive adsorption from background dissolved organic matter(DOM),present at substantially higher concentrations in mg L1.Interpreting the characteristics of competitive DOM is crucial in predicting OMP adsorption efficiencies across diverse natural waters.Molecular weight(MW),aromaticity,and polarity influence DOM competitiveness.Although the aromaticity-related metrics,such as UV254,of low MW DOM were proposed to correlate with DOM competitiveness,the method suffers from limitations in understanding the interplay of polarity and aromaticity in determining DOM competitiveness.Here,we elucidate the intricate influence of aromaticity and polarity in low MW DOM competition,spanning from a fraction level to a compound level,by employing direct sample injection liquid chromatography coupled with ultrahigh-resolution Fouriertransform ion cyclotron resonance mass spectrometry.Anion exchange resin pre-treatment eliminated 93%of UV254-active DOM,predominantly aromatic and polar DOM,and only minimally alleviated DOM competition.Molecular characterization revealed that nonpolar molecular formulas(constituting 26%PAC-adsorbable DOM)with medium aromaticity contributed more to the DOM competitiveness.Isomerlevel analysis indicated that the competitiveness of highly aromatic LMW DOM compounds was strongly counterbalanced by increased polarity.Strong aromaticity-derived p-p interaction cannot facilitate the competitive adsorption of hydrophilic DOM compounds.Our results underscore the constraints of depending solely on aromaticity-based approaches as the exclusive interpretive measure for DOM competitiveness.In a broader context,this study demonstrates an effect-oriented DOM analysis,elucidating counterbalancing interactions of DOM molecular properties from fraction to compound level.展开更多
To perform a systematic survey on the occurrence and removal of micropollutants during municipal wastewater treatment, 943 semi-volatile organic chemicals in 32 wastewater samples including influents of secondary trea...To perform a systematic survey on the occurrence and removal of micropollutants during municipal wastewater treatment, 943 semi-volatile organic chemicals in 32 wastewater samples including influents of secondary treatments, secondary effluents and final effluents(effluents of advanced treatments), which were collected from seven full-scale municipal wastewater treatment plants(MWTPs) in China, were examined by gas chromatography-mass spectrometry(GC-MS) coupled with an automated identification and quantification system with a database(AIQS-DB). In total, 196 and 145 chemicals were detected in secondary and final effluents, respectively. The majority of the total concentrations(average removal efficiency, 87.0%±5.9%) of the micropollutants were removed during secondary treatments. However, advanced treatments achieved different micropollutant removal extents from secondary effluents depending on the different treatment processes employed. Highly variable removal efficiencies of total concentrations(32.7%–99.3%) were observed among the different advanced processes. Among them,ozonation-based processes could remove 70.0%–80.9% of the total concentrations of studied micropollutants. The potentially harmful micropollutants, based on their detection frequency and concentration in secondary and final effluents, were polycyclic aromatic hydrocarbons(PAHs)(2-methylnaphthalene, fluoranthene, pyrene, naphthalene and phenanthrene), phosphorus flame retardants(tributyl phosphate(TBP), tris(2-chloroethyl)phosphate(TCEP) and tris(1,3-dichloro-2-propyl) phosphate(TDCP)), phthalates(bis(2-ethylhexyl)phthalate(DEHP)), benzothiazoles(benzothiazole,2-(methylthio)-benzothiazol, and 2(3H)-benzothiazolone) and phenol. This study indicated that the presence of considerable amounts of micropollutants in secondary effluent creates the need for suitable advanced treatment before their reuse.展开更多
The combination of hologram quantitative structure-activity relationship(HQSAR)and consensus modeling was employed to study the quantitative structure-property relationship(QSPR)model for calculating the aqueous hydro...The combination of hologram quantitative structure-activity relationship(HQSAR)and consensus modeling was employed to study the quantitative structure-property relationship(QSPR)model for calculating the aqueous hydroxyl radical oxidation reaction rate constants(kOH)of organic micropollutants(OMPs).Firstly,individual HQSAR model were established by using standard HQSAR method.The optimal individual HQSAR model was obtained while setting the parameter of fragment distinction and fragment size to“B”and“3~6”respectively.Secondly,consensus HQSAR model was established by building the regression model between the kOH and the hologram descriptors with consensus partial least-squares(cPLS)approach.The obtained individual and consensus HQSAR model were validated with a randomly selected external test set.The result of external test set validation demonstrates that both individual and consensus HQSAR model are available for predicting the kOH of OMPs.Compared with the optimal individual HQSAR model,the established consensus HQSAR model shows higher prediction accuracy and robustness.It is shown that the combination of HQSAR and consensus modeling is a practicable and promising method for studying and predicting the kOH of OMPs.展开更多
A rapid and effective method based on a novel permanent magnetic hypercrosslinked resin W150 was proposed for the removal of organic micropollutants in drinking water. W150 was prepared by suspension and post-crosslin...A rapid and effective method based on a novel permanent magnetic hypercrosslinked resin W150 was proposed for the removal of organic micropollutants in drinking water. W150 was prepared by suspension and post-crosslinking reaction and found to possess a high specific surface area of 1149.7 m^2· g^-1, a small particle size of 50 μm to 100 μm, and a saturation magnetization as high as 8 emu.g1. W150 was used to eliminate nitrofurazone (NFZ) and oxytetracycline (OTC) from drinking water compared with commercial adsorbents XAD-4 and F400D. The adsorption kinetics of NFZ and OTC onto the three adsorbents well fitted the pseudo-second-order equation (r 〉 0.972), and the adsorption isotherms were all well described by the Freundlich equation (r 〉 0.851). Results showed that the reduction in adsorbent size and the enlargement in sorbent pores both accelerated adsorption. Moreover, the effect of particle size on adsorption was more significant than that of pore width. Given that the smallest particle size and the highest specific surface area were possessed by W150, it had the fastest adsorption kinetics and largest adsorption capacity for NFZ (180 mg·g-1) and OTC (200mg·g- 1). For the adsorbents with dominant micropores, the sorption of large-sized adsorbates decreased because of the inaccessible micropores. The solution pH and ionic strength also influenced adsorption.展开更多
It is always highly pursued to develop efficient and durable catalysts for catalytic applications.Herein,intermetallic PdBi aerogels with tunable activity were prepared successfully via a surfactant-free spontaneous g...It is always highly pursued to develop efficient and durable catalysts for catalytic applications.Herein,intermetallic PdBi aerogels with tunable activity were prepared successfully via a surfactant-free spontaneous gelation process.The prepared PdBi aerogels have a three-dimensional high porous structure and plentiful active sites pervaded on the ultrathin interlinked nanowires network.These unique structures,as well as the synergistic effect between Pd and Bi,can accelerate mass and electron transfer,and improve the atom utilization ratio of Pd atoms to promote the catalytic efficiency.As a proofof-concept application,the optimized Pd_(2) Bi_(1) aerogels exhibit 4.2 and 6.2 times higher catalytic activity for the reduction of 4-nitrophenol(4-NP)and methylene blue(MB)than those of commercial Pd/C,respectively.With the introduction of non-noble metal of Bi,the cost of the resulted Pd Bi aerogels can be dropped signi ficantly while the catalytic capability of Pd Bi aerogel will be improved sharply.This strategy will bring good hints to rationally design fine catalysts for various applications.展开更多
Nowadays the protection of the marine environment raises increasing academic and public attention.The issue of organic micropollutants is of equally high importance for the marine ecosystems.Maritime vessels are consi...Nowadays the protection of the marine environment raises increasing academic and public attention.The issue of organic micropollutants is of equally high importance for the marine ecosystems.Maritime vessels are considered to significant sources of micropollutants especially if the ship carries many passengers,which is often true for cruise ships which frequent attractive and sensitive sea areas.The emission pathways for micropollutants include wastewater discharges and sewage sludge disposal.The findings of the German research and development project NAUTEK contribute to bridging the knowledge gap about micropollutant emissions from cruise ships.As expected,micropollutants were detected in both the blackwater and greywater on board,emitted from either the passengers or certain ship operations.In total,16 out of 21 target substances were detected.Peak concentrations of pharmaceuticals could be found mainly in blackwater(peak conc.Carbamazepine 3.9 mg/L,Ibuprofen 29 mg/L,Diclofenac 0.04 mg/L),while greywater is mainly characterized by substances such as ointment residues,UV-filters and flame retardants(peak conc.Diclofenac 0.65 mg/L,Bisphenol A 8 mg/L,Tris(1-chloro-2-propyl)phosphate 136 mg/L).Further analyses suggest a gradual removal of the micropollutants by the onboard MBR plant(MBR effluent peak conc.Carbamazepine 0.47 mg/L,Ibuprofen 6.8 mg/L,Diclofenac 0.3 mg/L).Findings of this research provide a critical stepstone for shaping technical solutions for onboard micropollutants removal and water resource recycling.展开更多
基金the National Natural Science Foundation of China (No.50538090)the National Basic Research Program (973) of China (No.2007CB407301)ST Program of Beijing Municipality (No.D0706007040291-01).
文摘Organic micropollutants,with high toxicity and environmental concern,are present in the landfill leachate at much lower levels than total organic constituents (chemical oxygen demand (COD),biochemical oxygen demand (BOD),or total organic carbon (TOC)),and few has been known for their behaviors in different treatment processes.In this study,occurrence and removal of 17 organochlorine pesticides (OCPs),16 polycyclic aromatic hydrocarbons (PAHs),and technical 4-nonylphenol (4-NP) in landfill leachate in a comb...
基金supported by the National Key R&D Program of China(2022YFC3203701)the National Natural Science Foundation of China(52070185)+1 种基金the Fellowship of China Postdoctoral Science Foundation(2022M723320)the Department of Water Management of TU Delft.
文摘Activated carbon is employed for the adsorption of organic micropollutants(OMPs)from water,typically present in concentrations ranging from ng L1 to mg L1.However,the efficacy of OMP removal is considerably deteriorated due to competitive adsorption from background dissolved organic matter(DOM),present at substantially higher concentrations in mg L1.Interpreting the characteristics of competitive DOM is crucial in predicting OMP adsorption efficiencies across diverse natural waters.Molecular weight(MW),aromaticity,and polarity influence DOM competitiveness.Although the aromaticity-related metrics,such as UV254,of low MW DOM were proposed to correlate with DOM competitiveness,the method suffers from limitations in understanding the interplay of polarity and aromaticity in determining DOM competitiveness.Here,we elucidate the intricate influence of aromaticity and polarity in low MW DOM competition,spanning from a fraction level to a compound level,by employing direct sample injection liquid chromatography coupled with ultrahigh-resolution Fouriertransform ion cyclotron resonance mass spectrometry.Anion exchange resin pre-treatment eliminated 93%of UV254-active DOM,predominantly aromatic and polar DOM,and only minimally alleviated DOM competition.Molecular characterization revealed that nonpolar molecular formulas(constituting 26%PAC-adsorbable DOM)with medium aromaticity contributed more to the DOM competitiveness.Isomerlevel analysis indicated that the competitiveness of highly aromatic LMW DOM compounds was strongly counterbalanced by increased polarity.Strong aromaticity-derived p-p interaction cannot facilitate the competitive adsorption of hydrophilic DOM compounds.Our results underscore the constraints of depending solely on aromaticity-based approaches as the exclusive interpretive measure for DOM competitiveness.In a broader context,this study demonstrates an effect-oriented DOM analysis,elucidating counterbalancing interactions of DOM molecular properties from fraction to compound level.
基金supported by the Major Science and Technology Program for Water Pollution Control and Treatment in China(No.2017ZX07106005)
文摘To perform a systematic survey on the occurrence and removal of micropollutants during municipal wastewater treatment, 943 semi-volatile organic chemicals in 32 wastewater samples including influents of secondary treatments, secondary effluents and final effluents(effluents of advanced treatments), which were collected from seven full-scale municipal wastewater treatment plants(MWTPs) in China, were examined by gas chromatography-mass spectrometry(GC-MS) coupled with an automated identification and quantification system with a database(AIQS-DB). In total, 196 and 145 chemicals were detected in secondary and final effluents, respectively. The majority of the total concentrations(average removal efficiency, 87.0%±5.9%) of the micropollutants were removed during secondary treatments. However, advanced treatments achieved different micropollutant removal extents from secondary effluents depending on the different treatment processes employed. Highly variable removal efficiencies of total concentrations(32.7%–99.3%) were observed among the different advanced processes. Among them,ozonation-based processes could remove 70.0%–80.9% of the total concentrations of studied micropollutants. The potentially harmful micropollutants, based on their detection frequency and concentration in secondary and final effluents, were polycyclic aromatic hydrocarbons(PAHs)(2-methylnaphthalene, fluoranthene, pyrene, naphthalene and phenanthrene), phosphorus flame retardants(tributyl phosphate(TBP), tris(2-chloroethyl)phosphate(TCEP) and tris(1,3-dichloro-2-propyl) phosphate(TDCP)), phthalates(bis(2-ethylhexyl)phthalate(DEHP)), benzothiazoles(benzothiazole,2-(methylthio)-benzothiazol, and 2(3H)-benzothiazolone) and phenol. This study indicated that the presence of considerable amounts of micropollutants in secondary effluent creates the need for suitable advanced treatment before their reuse.
基金supported by the National Natural Science Foundation of China(No.21775118)Shaanxi Natural Science Basic Research Project(No.2018JM2018)+2 种基金Youth Innovation Team of Shaanxi Universities(No.2019.21)Young Outstanding Talent Support Program of Shaanxi UniversitiesXi’an Shiyou University Youth Research and Innovation Team Construction Plan(No.2019QNKYCXTD17),and Xi’an Shiyou University Graduate Innovation and Practice Ability Training Project(No.YCS19211016)。
文摘The combination of hologram quantitative structure-activity relationship(HQSAR)and consensus modeling was employed to study the quantitative structure-property relationship(QSPR)model for calculating the aqueous hydroxyl radical oxidation reaction rate constants(kOH)of organic micropollutants(OMPs).Firstly,individual HQSAR model were established by using standard HQSAR method.The optimal individual HQSAR model was obtained while setting the parameter of fragment distinction and fragment size to“B”and“3~6”respectively.Secondly,consensus HQSAR model was established by building the regression model between the kOH and the hologram descriptors with consensus partial least-squares(cPLS)approach.The obtained individual and consensus HQSAR model were validated with a randomly selected external test set.The result of external test set validation demonstrates that both individual and consensus HQSAR model are available for predicting the kOH of OMPs.Compared with the optimal individual HQSAR model,the established consensus HQSAR model shows higher prediction accuracy and robustness.It is shown that the combination of HQSAR and consensus modeling is a practicable and promising method for studying and predicting the kOH of OMPs.
文摘A rapid and effective method based on a novel permanent magnetic hypercrosslinked resin W150 was proposed for the removal of organic micropollutants in drinking water. W150 was prepared by suspension and post-crosslinking reaction and found to possess a high specific surface area of 1149.7 m^2· g^-1, a small particle size of 50 μm to 100 μm, and a saturation magnetization as high as 8 emu.g1. W150 was used to eliminate nitrofurazone (NFZ) and oxytetracycline (OTC) from drinking water compared with commercial adsorbents XAD-4 and F400D. The adsorption kinetics of NFZ and OTC onto the three adsorbents well fitted the pseudo-second-order equation (r 〉 0.972), and the adsorption isotherms were all well described by the Freundlich equation (r 〉 0.851). Results showed that the reduction in adsorbent size and the enlargement in sorbent pores both accelerated adsorption. Moreover, the effect of particle size on adsorption was more significant than that of pore width. Given that the smallest particle size and the highest specific surface area were possessed by W150, it had the fastest adsorption kinetics and largest adsorption capacity for NFZ (180 mg·g-1) and OTC (200mg·g- 1). For the adsorbents with dominant micropores, the sorption of large-sized adsorbates decreased because of the inaccessible micropores. The solution pH and ionic strength also influenced adsorption.
基金the financial support from the National Natural Science Foundation of China(Nos.21245007 and 81000976)the Natural Science Foundation of Shandong Province(No.ZR2017MB017)+1 种基金Scientific Start-up Research Fund of Chengdu University of Information Technology(No.KYTZ201714)the open fund of Innovation&Application Engineering Research Center for Mesoporous Materials of Shanxi Province(No.MMIA2019001)。
文摘It is always highly pursued to develop efficient and durable catalysts for catalytic applications.Herein,intermetallic PdBi aerogels with tunable activity were prepared successfully via a surfactant-free spontaneous gelation process.The prepared PdBi aerogels have a three-dimensional high porous structure and plentiful active sites pervaded on the ultrathin interlinked nanowires network.These unique structures,as well as the synergistic effect between Pd and Bi,can accelerate mass and electron transfer,and improve the atom utilization ratio of Pd atoms to promote the catalytic efficiency.As a proofof-concept application,the optimized Pd_(2) Bi_(1) aerogels exhibit 4.2 and 6.2 times higher catalytic activity for the reduction of 4-nitrophenol(4-NP)and methylene blue(MB)than those of commercial Pd/C,respectively.With the introduction of non-noble metal of Bi,the cost of the resulted Pd Bi aerogels can be dropped signi ficantly while the catalytic capability of Pd Bi aerogel will be improved sharply.This strategy will bring good hints to rationally design fine catalysts for various applications.
基金This work was supported by the German Federal Ministry of Economic Affairs and Energy(BMWi)in the Project NAUTEK Sustainable Wastewater Treatment and Recycling on Cruise Liners(Grant No.03SX360)upon a decision of the German Bundestag.We appreciate the support from the funding agency for the possibility to carry out the work described here.We also thank the ships'crews for their great support.
文摘Nowadays the protection of the marine environment raises increasing academic and public attention.The issue of organic micropollutants is of equally high importance for the marine ecosystems.Maritime vessels are considered to significant sources of micropollutants especially if the ship carries many passengers,which is often true for cruise ships which frequent attractive and sensitive sea areas.The emission pathways for micropollutants include wastewater discharges and sewage sludge disposal.The findings of the German research and development project NAUTEK contribute to bridging the knowledge gap about micropollutant emissions from cruise ships.As expected,micropollutants were detected in both the blackwater and greywater on board,emitted from either the passengers or certain ship operations.In total,16 out of 21 target substances were detected.Peak concentrations of pharmaceuticals could be found mainly in blackwater(peak conc.Carbamazepine 3.9 mg/L,Ibuprofen 29 mg/L,Diclofenac 0.04 mg/L),while greywater is mainly characterized by substances such as ointment residues,UV-filters and flame retardants(peak conc.Diclofenac 0.65 mg/L,Bisphenol A 8 mg/L,Tris(1-chloro-2-propyl)phosphate 136 mg/L).Further analyses suggest a gradual removal of the micropollutants by the onboard MBR plant(MBR effluent peak conc.Carbamazepine 0.47 mg/L,Ibuprofen 6.8 mg/L,Diclofenac 0.3 mg/L).Findings of this research provide a critical stepstone for shaping technical solutions for onboard micropollutants removal and water resource recycling.