The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2...The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2 FTS were tested on the Ti/SnO2–Sb2O5–Bi2O3anode. The effects of current density,potential,and supporting electrolyte on the degradation of 6：2 FTS were evaluated. Experimental results showed that 6：2 FTS was more easily degraded than PFOS on the Ti/SnO2–Sb2O5–Bi2O3anode. At a low current density of 1.42 mA/cm2,6：2 FTS was not degraded on Ti/SnO2–Sb2O5–Bi2O3,while the degradation ratio increased when the current density ranged from 4.25 to 6.80 mA/cm2. The degradation of 6：2 FTS at current density of 6.80 mA/cm2 followed pseudo first-order kinetics with the rate constant of 0.074 hr-1. The anodic potential played an important role in the degradation of 6：2 FTS,and the pseudo first-order rate constants increased with the potential. The surface of Ti/SnO2–Sb2O5–Bi2O3was contaminated after electrolysis at constant potential of 3 V,while the fouling phenomenon was not observed at 5 V. The fouled anode could be regenerated by incinerating at 600°C. The intermediates detected by ultra-performance liquid chromatography coupled with a triple-stage quadrupole mass spectrometer（UPLC–MS/MS） were shorter chain perfluorocarboxylic acids. The 6：2 FTS was first attacked by hydroxyl radical,and then formed perfluorinated carboxylates,which decarboxylated and removed CF2 units to yield shorter-chain perfluorocarboxylic acids.展开更多
To meet the rapidly growing global demand for aquaculture products,large amounts of antibiotics were used in aquaculture,which might accelerate the evolution of antibiotic-resistant bacteria(ARB)and the propagation of...To meet the rapidly growing global demand for aquaculture products,large amounts of antibiotics were used in aquaculture,which might accelerate the evolution of antibiotic-resistant bacteria(ARB)and the propagation of antibiotic genes(ARGs).In our research,we revealed the ARGs profiles,their co-occurrence with mobile genetic elements(MGEs),and potential hosts in sediments of a crab pond wastewater purification system based on metagenomic analysis.The residual antibiotic seems to increase the propagation of ARGs in the crab pond,but there was no clear relationship between a given antibiotic type and the corresponding resistance genes.The effect of aquaculture on sediment was not as profound as that of other anthropogentic activities,but increased the relative abundance of sulfon-amide resistance gene.A higher abundance of MGEs,especially plasmid,increased the po-tential ARGs dissemination risk in crab and purification ponds.Multidrug and sulfonamide resistance genes had greater potential to transfer because they were more frequently carried by MGEs.The horizontal gene transfer was likely to occur among a variety of microorgan-isms,and various ARGs hosts including Pseudomonas,Acinetobacter,Escherichia,and Klebsiella were identified.Bacterial community influenced the composition of ARG hosts,and Pro-teobacteria was the predominant hosts.Overall,our study provides novel insights into the environmental risk of ARGs in sediments of aquaculture wastewater treatment system.展开更多
The authors regret<We found an error in Eq.(2)of J.Environ.Sci.,2022,113,345-355(Ncell was obtained from the calculation of ARGs-OAP software,so it doesn’t affect the subsequent results).Eq.(2)is revised as follow...The authors regret<We found an error in Eq.(2)of J.Environ.Sci.,2022,113,345-355(Ncell was obtained from the calculation of ARGs-OAP software,so it doesn’t affect the subsequent results).Eq.(2)is revised as follows(Yang et al.,2016).展开更多
Rapidly increasing concentration of CO2 in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO2 capture from the anthropogenic sources...Rapidly increasing concentration of CO2 in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO2 capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and C02 adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO2 adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO2 adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine （PEI） on the different porous materials were introduced in terms of preparation method and adsorption perfor- mance as well as their advantages and disadvantages for CO2 adsorption. In the last section, the issues and prospect of solid adsorbents for CO2 adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of acti- vated carbons and amine-modified adsorbents for CO2 capture.展开更多
The Stockholm Convention on persistent organic pollutants （POPs） was adopted in 2001. This year is the 10th anniversary of the adoption of the Convention. Until now, 22 chemicals or chemical categories have been lis...The Stockholm Convention on persistent organic pollutants （POPs） was adopted in 2001. This year is the 10th anniversary of the adoption of the Convention. Until now, 22 chemicals or chemical categories have been listed as POPs in the Stockholm Convention. The POPs Research Center was established in Tsinghua University in the same year when the Convention was adopted. In the last ten years, much work has been done by Chinese researchers to understand the environ- mental risk of POPs in China. This article aims to review the recent research progress of our POPs Research Center and some other Chinese researchers＇ studies in addressing the environmental risk of POPs, including the priority screening and inventory study of POPs, monitoring and modeling of POPs pollution and exposure, and environ- mental risk assessment and modeling of POPs. Although great advances in addressing the environmental risk of POPs have been made in recent years, we are still facing quite a few problems, such as data scarcity and uncertainty in environmental risk assessment of POPs. The study on the effect of POPs mixtures is in its infancy and currently POPs are usually assessed from legal perspective by risk assessment of single chemicals. These problems should be well addressed by further efforts. Further studies should also be taken in future to study environment risk of POPs by considering aspects of coupled dynamics between climate processes and POPs. Such sound scientific, riskbased information can support decision-making aiming to effectively minimize the risk level of POPs.展开更多
Perfluorooctane sulfonate(PFOS),as a potential persistent organic pollutant,has been widely detected in water environments,and has become a great concern in recent years.PFOS is very stable and difficult to decompose ...Perfluorooctane sulfonate(PFOS),as a potential persistent organic pollutant,has been widely detected in water environments,and has become a great concern in recent years.PFOS is very stable and difficult to decompose using conventional techniques.Sorption may be an attractive method to remove it from water.In this study,the molecularly imprinted polymer(MIP)adsorbents were prepared through the polymerization of 4-vinylpyridine under different preparation conditions in order to remove perfluorooctane sulfonate(PFOS)from water.The MIP adsorbents using perfluorooctanoic acid(PFOA)as the template had good imprinting effects and could selectively remove PFOS from aqueous solution.The sorption behaviors including sorption kinetics,isotherms,and effect of pH,salt,and competitive anions were investigated.Experimental results showed that the sorption of PFOS on the MIP adsorbents was very fast,pHdependent,and highly selective.The achieved fast sorption equilibrium within 1 h was attributed to the surface sorption on the fine adsorbents.The sorption isotherms showed that the sorption selectivity of PFOS on the MIP adsorbents decreased at high PFOS concentrations,which may be due to the double-layer sorption and the formation of PFOS micelles on the sorbent surface.The sorption of PFOS on the MIP adsorbents was mainly dominated by the electrostatic interaction between the protonated vinylpyridine on the adsorbent surface and the anionic PFOS.The prepared MIP adsorbents can potentially be applied in water and wastewater treatment for selective removal of PFOS.展开更多
As a party of the Stockholm Convention on Per-sistent Organic Pollutants,China must submit its national implementation plan(NIP)for this convention.The strategy and action plan for reducing the release of dioxins in C...As a party of the Stockholm Convention on Per-sistent Organic Pollutants,China must submit its national implementation plan(NIP)for this convention.The strategy and action plan for reducing the release of dioxins in China are the most important components of the NIP.Three prob-lems are key points for developing such strategy and action plan-what are the key sources for applying the best avail-able technology/best environmental practice(BAT/BEP)to reduce the release of dioxins?How about the capacity for reducing the dioxins release from the key sources?Where are the areas of priority for applying BAT/BEP?This paper shows the efforts towards the solution of these problems.The list of key sources covering about half of the total dioxins release was determined considering four criteria.The capacity of key sources were estimated based on the difference between the emission factor corresponding to the actual situation in 2004 and that corresponding to the scenario that all key sources have been applied BAT/BEP to reduce the dioxins release.The priority analysis using the geographical information system(GIS)tool has revealed that eastern provinces should be of high priority in the future reduction activities of dioxins release in China.展开更多
Polymer thermal recycling for hydrogen production is a promising process to recover such precious element from plastic waste. In the present work a simple but efficacious high energy milling pretreatment is proposed t...Polymer thermal recycling for hydrogen production is a promising process to recover such precious element from plastic waste. In the present work a simple but efficacious high energy milling pretreatment is proposed to boost H2 generation during polyethylene gasification. The polymer is comilled with calcium and nickel hydroxides and then it is subjected to thermal treatment. Results demonstrate the key role played by the calcium hydroxide that significantly ameliorates hydrogen production. It reacts in solid state with the polyethylene to fonn directly carbonate and hydrogen. In this way, the CO2 is immediately captured in solid fonn, thus shifting the equilibrium toward H2 generation and obtaining high production rate (>25 L/mol CH2). In addition, high amounts of the hydroxide prevent excessive methane fonnation, so the gas product is almost pure hydrogen (~95%).展开更多
Polyethylenimine （PEI）-modified chitosan was prepared and used to remove clofibric acid （CA） from aqueous solution. PEI was chemically grafted on the porous chitosan through a crosslinking reaction, and the effect...Polyethylenimine （PEI）-modified chitosan was prepared and used to remove clofibric acid （CA） from aqueous solution. PEI was chemically grafted on the porous chitosan through a crosslinking reaction, and the effects of PEI concentration and reaction time in the preparation on the adsorption of clofibric acid were optimized. Scanning electron microscopy （SEM） showed that PEI macromolecules were uniformly grafted on the porous chitosan, and the analysis of pore size distribution indicated that more mesopores were formed due to the crosslinking of PEI molecules in the macropores of chitosan. The PEI-modified chitosan had fast adsorption for CA within the initial 5 h, while this adsorbent exhibited an adsorption capacity of 349 mg· g^-1 for CA at pH 5.0 according to the Langmuir fitting, higher than 213 mg· g^-1 on the porous chitosan. The CA adsorption on the PEI- modified chitosan was pH-dependent, and the maximum adsorption was achieved at pH 4.0. Based on the surface charge analysis and comparison of different pharmaceu- ticals adsorption, electrostatic interaction dominated the sorption of CA on the PEI-modified chitosan. The PEI- modified chitosan has a potential application for the removal of some anionic rnicropollutants from water or wastewater.展开更多
Homolog and congener profiles of polychlori- nated biphenyls （PCBs）, polychlorinated dibenzo-p- dioxins （PCDDs） and polychlorinated dibenzofurans （PCDFs） in commercial PCBs formulations are useful information fo...Homolog and congener profiles of polychlori- nated biphenyls （PCBs）, polychlorinated dibenzo-p- dioxins （PCDDs） and polychlorinated dibenzofurans （PCDFs） in commercial PCBs formulations are useful information for the source appointment of PCBs contam- ination as well as the risk assessment caused by potential exposure. Dielectric oil （ASKAREL Nr 1740） in an imported transformer found in China was sampled and analyzed by isotope dilution technology using high resolution gas chromatography-high resolution mass spectrometry （HRGC/HRMS）. The detailed homolog and congener profiles of PCBs obtained were compared with those of known Aroclor formulations. High similarity in the homolog profile between the oil sample and Aroclor 1260was found, with the hexachlorinated and hepta- chlorinated biphenyls accounting for more than 80.2% of the total PCBs concentration. Severn indicator PCBs contribute about 30%, while 12 PCB congeners （i.e., # 153, #143, #168, #180, #149, #165, #138, #170, #190, #187, #174, #181） account for more than 50% of the total PCB concentrations. Total concentration ofPCDDs, PCDFs and dioxin-like PCBs （DL-PCBs） was found to be 740 ng TEQ/g, of which 620 ng TEQ/g came from DL-PCBs. The contribution of PCDDs to the total TEQ was neglectable. The concentration of PCDFs homologs follows the order of OCDF 〉 HxCDFs 〉 HpCDFs 〉 PeCDFs 〉 TeCDFs, which is in consistence with the previous study on Aroclor 1260. Three DL-PCBs congeners （i.e., #118, #156, #157） accounted for 77% of the total concentration of DL-PCBs, also they contribute 72% in the TEQ caused by DL-PCBs.展开更多
Three adsorbents including TiO_(2),Ti-Ce,and Ti-La hybrid oxides were prepared to remove fluoride from aqueous solution.The Ti-Ce and Ti-La hybrid adsorbents obtained by the hydrolysis-precipitation method had much hi...Three adsorbents including TiO_(2),Ti-Ce,and Ti-La hybrid oxides were prepared to remove fluoride from aqueous solution.The Ti-Ce and Ti-La hybrid adsorbents obtained by the hydrolysis-precipitation method had much higher sorption capacity for fluoride than the TiO_(2) adsorbent prepared through hydrolysis.Rare earth(Ce and La)oxides and TiO_(2) exhibited a synergistic effect in the hybrid adsorbents for fluoride sorption.The sorption equilibrium of fluoride on the three adsorbents was achieved within 4 h,and the pseudo-second-order model described the sorption kinetics well.The sorption isotherms fitted the Langmuir model well,and the adsorption capacities of fluoride on the Ti-Ce and Ti-La adsorbents were about 9.6 and 15.1 mg·g^(-1),respectively,at the equilibrium fluoride concentration of 1.0 mg·L^(-1),much higher than the 1.7 mg·g^(-1) on the TiO_(2).The sorption capacities of fluoride on the three adsorbents decreased significantly when the solution pH increased from 3 to 9.5.The electrostatic interaction played an important role in fluoride removal by the three adsorbents,and Fourier transform infrared(FTIR)analysis indicated that the hydroxyl groups on the adsorbent surface were involved in fluoride adsorption.展开更多
Ozonation has been proved to be a promising approach for eliminating emerging pollutants in wastewater.In previous studies,emerging pollutants including diverse pharmaceuticals were found to exhibit significantly diff...Ozonation has been proved to be a promising approach for eliminating emerging pollutants in wastewater.In previous studies,emerging pollutants including diverse pharmaceuticals were found to exhibit significantly different ozonation reactivity.However,how the structural differences of emerging pollutants determine ozonation reactivity and mechanisms are still ambiguous.In this work,ozonation of dimethylaminophenazone(DMP)and acetylaminophenazone(AAA)with the same parent structure of phenazone but different substitution groups was investigated,in order to probe influencing mechanisms of structural differences on ozonation reactivity.Results show that DMP reacts with ozone and HOalmost 2 and 1 order of magnitude faster than AAA,respectively.At pH 8,HO· accelerates ozonation of DMP,but decreases ozonation of AAA.Competition simultaneously decreases degradation rate of the two phenazones,but effects on AAA are more significant than that on DMP.According to theoretical calculation results,differences in ozonation reactivity and mechanisms of the two phenazones can be mainly attributed to different substitution groups.The dimethylamino group in the structure of DMP increases the ozonation reactivity of phenazone by increasing reaction orbital energies and altering reaction sites,while the acetylamino group in the structure of AAA decreases the reaction orbital energy and therefore lowers the reactivity.展开更多
基金supported by the National Natural Science Foundation of China (No.21307036)the National High-Tech Research and Development Program of China (No.2013AA062705)the National Key Scientific and Technological Project for Water Pollution Control and Management (Nos.2012ZX07206-002,2012ZX07206-003)
文摘The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2 FTS were tested on the Ti/SnO2–Sb2O5–Bi2O3anode. The effects of current density,potential,and supporting electrolyte on the degradation of 6：2 FTS were evaluated. Experimental results showed that 6：2 FTS was more easily degraded than PFOS on the Ti/SnO2–Sb2O5–Bi2O3anode. At a low current density of 1.42 mA/cm2,6：2 FTS was not degraded on Ti/SnO2–Sb2O5–Bi2O3,while the degradation ratio increased when the current density ranged from 4.25 to 6.80 mA/cm2. The degradation of 6：2 FTS at current density of 6.80 mA/cm2 followed pseudo first-order kinetics with the rate constant of 0.074 hr-1. The anodic potential played an important role in the degradation of 6：2 FTS,and the pseudo first-order rate constants increased with the potential. The surface of Ti/SnO2–Sb2O5–Bi2O3was contaminated after electrolysis at constant potential of 3 V,while the fouling phenomenon was not observed at 5 V. The fouled anode could be regenerated by incinerating at 600°C. The intermediates detected by ultra-performance liquid chromatography coupled with a triple-stage quadrupole mass spectrometer（UPLC–MS/MS） were shorter chain perfluorocarboxylic acids. The 6：2 FTS was first attacked by hydroxyl radical,and then formed perfluorinated carboxylates,which decarboxylated and removed CF2 units to yield shorter-chain perfluorocarboxylic acids.
基金supported by Unité de Catalyse et Chimie du Solide (UCCS)sponsor of scholarship: China scholarship council and School of Environment, Tsinghua University
基金This work was financially supported by the National Natural Science Foundation of China(No.51778006)the High-performance Computing Platform of Peking University。
文摘To meet the rapidly growing global demand for aquaculture products,large amounts of antibiotics were used in aquaculture,which might accelerate the evolution of antibiotic-resistant bacteria(ARB)and the propagation of antibiotic genes(ARGs).In our research,we revealed the ARGs profiles,their co-occurrence with mobile genetic elements(MGEs),and potential hosts in sediments of a crab pond wastewater purification system based on metagenomic analysis.The residual antibiotic seems to increase the propagation of ARGs in the crab pond,but there was no clear relationship between a given antibiotic type and the corresponding resistance genes.The effect of aquaculture on sediment was not as profound as that of other anthropogentic activities,but increased the relative abundance of sulfon-amide resistance gene.A higher abundance of MGEs,especially plasmid,increased the po-tential ARGs dissemination risk in crab and purification ponds.Multidrug and sulfonamide resistance genes had greater potential to transfer because they were more frequently carried by MGEs.The horizontal gene transfer was likely to occur among a variety of microorgan-isms,and various ARGs hosts including Pseudomonas,Acinetobacter,Escherichia,and Klebsiella were identified.Bacterial community influenced the composition of ARG hosts,and Pro-teobacteria was the predominant hosts.Overall,our study provides novel insights into the environmental risk of ARGs in sediments of aquaculture wastewater treatment system.
文摘The authors regret<We found an error in Eq.(2)of J.Environ.Sci.,2022,113,345-355(Ncell was obtained from the calculation of ARGs-OAP software,so it doesn’t affect the subsequent results).Eq.(2)is revised as follows(Yang et al.,2016).
文摘Rapidly increasing concentration of CO2 in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO2 capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and C02 adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO2 adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO2 adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine （PEI） on the different porous materials were introduced in terms of preparation method and adsorption perfor- mance as well as their advantages and disadvantages for CO2 adsorption. In the last section, the issues and prospect of solid adsorbents for CO2 adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of acti- vated carbons and amine-modified adsorbents for CO2 capture.
文摘The Stockholm Convention on persistent organic pollutants （POPs） was adopted in 2001. This year is the 10th anniversary of the adoption of the Convention. Until now, 22 chemicals or chemical categories have been listed as POPs in the Stockholm Convention. The POPs Research Center was established in Tsinghua University in the same year when the Convention was adopted. In the last ten years, much work has been done by Chinese researchers to understand the environ- mental risk of POPs in China. This article aims to review the recent research progress of our POPs Research Center and some other Chinese researchers＇ studies in addressing the environmental risk of POPs, including the priority screening and inventory study of POPs, monitoring and modeling of POPs pollution and exposure, and environ- mental risk assessment and modeling of POPs. Although great advances in addressing the environmental risk of POPs have been made in recent years, we are still facing quite a few problems, such as data scarcity and uncertainty in environmental risk assessment of POPs. The study on the effect of POPs mixtures is in its infancy and currently POPs are usually assessed from legal perspective by risk assessment of single chemicals. These problems should be well addressed by further efforts. Further studies should also be taken in future to study environment risk of POPs by considering aspects of coupled dynamics between climate processes and POPs. Such sound scientific, riskbased information can support decision-making aiming to effectively minimize the risk level of POPs.
基金This work was supported by the National Natural Science Foundation of China(Grant No.50608045)the special fund of State Key Joint Laboratory of Environment Simulation and Pollution(Grant No.08Z04ESPCT)the National Outstanding Youth Foundation of China(Grant No.50625823).
文摘Perfluorooctane sulfonate(PFOS),as a potential persistent organic pollutant,has been widely detected in water environments,and has become a great concern in recent years.PFOS is very stable and difficult to decompose using conventional techniques.Sorption may be an attractive method to remove it from water.In this study,the molecularly imprinted polymer(MIP)adsorbents were prepared through the polymerization of 4-vinylpyridine under different preparation conditions in order to remove perfluorooctane sulfonate(PFOS)from water.The MIP adsorbents using perfluorooctanoic acid(PFOA)as the template had good imprinting effects and could selectively remove PFOS from aqueous solution.The sorption behaviors including sorption kinetics,isotherms,and effect of pH,salt,and competitive anions were investigated.Experimental results showed that the sorption of PFOS on the MIP adsorbents was very fast,pHdependent,and highly selective.The achieved fast sorption equilibrium within 1 h was attributed to the surface sorption on the fine adsorbents.The sorption isotherms showed that the sorption selectivity of PFOS on the MIP adsorbents decreased at high PFOS concentrations,which may be due to the double-layer sorption and the formation of PFOS micelles on the sorbent surface.The sorption of PFOS on the MIP adsorbents was mainly dominated by the electrostatic interaction between the protonated vinylpyridine on the adsorbent surface and the anionic PFOS.The prepared MIP adsorbents can potentially be applied in water and wastewater treatment for selective removal of PFOS.
基金This research was supported by funding provided by the Stockholm Convention Implementing Office at State Environmental Protection Administration(CIO/SEPA).
文摘As a party of the Stockholm Convention on Per-sistent Organic Pollutants,China must submit its national implementation plan(NIP)for this convention.The strategy and action plan for reducing the release of dioxins in China are the most important components of the NIP.Three prob-lems are key points for developing such strategy and action plan-what are the key sources for applying the best avail-able technology/best environmental practice(BAT/BEP)to reduce the release of dioxins?How about the capacity for reducing the dioxins release from the key sources?Where are the areas of priority for applying BAT/BEP?This paper shows the efforts towards the solution of these problems.The list of key sources covering about half of the total dioxins release was determined considering four criteria.The capacity of key sources were estimated based on the difference between the emission factor corresponding to the actual situation in 2004 and that corresponding to the scenario that all key sources have been applied BAT/BEP to reduce the dioxins release.The priority analysis using the geographical information system(GIS)tool has revealed that eastern provinces should be of high priority in the future reduction activities of dioxins release in China.
文摘Polymer thermal recycling for hydrogen production is a promising process to recover such precious element from plastic waste. In the present work a simple but efficacious high energy milling pretreatment is proposed to boost H2 generation during polyethylene gasification. The polymer is comilled with calcium and nickel hydroxides and then it is subjected to thermal treatment. Results demonstrate the key role played by the calcium hydroxide that significantly ameliorates hydrogen production. It reacts in solid state with the polyethylene to fonn directly carbonate and hydrogen. In this way, the CO2 is immediately captured in solid fonn, thus shifting the equilibrium toward H2 generation and obtaining high production rate (>25 L/mol CH2). In addition, high amounts of the hydroxide prevent excessive methane fonnation, so the gas product is almost pure hydrogen (~95%).
基金Acknowledgements This research was supported by the National Natural Science Foundation of China （Grant No. 51078217）, Special Fund of State Key Joint Laboratory of Environment Simulation and Pollution （No. 12L02ESPC）, and the Collaborative Innovation Center for Regional Environmental Quality. Additionally, the analytical work was supported by the Laboratory Fund of Tsinghua University.
文摘Polyethylenimine （PEI）-modified chitosan was prepared and used to remove clofibric acid （CA） from aqueous solution. PEI was chemically grafted on the porous chitosan through a crosslinking reaction, and the effects of PEI concentration and reaction time in the preparation on the adsorption of clofibric acid were optimized. Scanning electron microscopy （SEM） showed that PEI macromolecules were uniformly grafted on the porous chitosan, and the analysis of pore size distribution indicated that more mesopores were formed due to the crosslinking of PEI molecules in the macropores of chitosan. The PEI-modified chitosan had fast adsorption for CA within the initial 5 h, while this adsorbent exhibited an adsorption capacity of 349 mg· g^-1 for CA at pH 5.0 according to the Langmuir fitting, higher than 213 mg· g^-1 on the porous chitosan. The CA adsorption on the PEI- modified chitosan was pH-dependent, and the maximum adsorption was achieved at pH 4.0. Based on the surface charge analysis and comparison of different pharmaceu- ticals adsorption, electrostatic interaction dominated the sorption of CA on the PEI-modified chitosan. The PEI- modified chitosan has a potential application for the removal of some anionic rnicropollutants from water or wastewater.
文摘Homolog and congener profiles of polychlori- nated biphenyls （PCBs）, polychlorinated dibenzo-p- dioxins （PCDDs） and polychlorinated dibenzofurans （PCDFs） in commercial PCBs formulations are useful information for the source appointment of PCBs contam- ination as well as the risk assessment caused by potential exposure. Dielectric oil （ASKAREL Nr 1740） in an imported transformer found in China was sampled and analyzed by isotope dilution technology using high resolution gas chromatography-high resolution mass spectrometry （HRGC/HRMS）. The detailed homolog and congener profiles of PCBs obtained were compared with those of known Aroclor formulations. High similarity in the homolog profile between the oil sample and Aroclor 1260was found, with the hexachlorinated and hepta- chlorinated biphenyls accounting for more than 80.2% of the total PCBs concentration. Severn indicator PCBs contribute about 30%, while 12 PCB congeners （i.e., # 153, #143, #168, #180, #149, #165, #138, #170, #190, #187, #174, #181） account for more than 50% of the total PCB concentrations. Total concentration ofPCDDs, PCDFs and dioxin-like PCBs （DL-PCBs） was found to be 740 ng TEQ/g, of which 620 ng TEQ/g came from DL-PCBs. The contribution of PCDDs to the total TEQ was neglectable. The concentration of PCDFs homologs follows the order of OCDF 〉 HxCDFs 〉 HpCDFs 〉 PeCDFs 〉 TeCDFs, which is in consistence with the previous study on Aroclor 1260. Three DL-PCBs congeners （i.e., #118, #156, #157） accounted for 77% of the total concentration of DL-PCBs, also they contribute 72% in the TEQ caused by DL-PCBs.
文摘Three adsorbents including TiO_(2),Ti-Ce,and Ti-La hybrid oxides were prepared to remove fluoride from aqueous solution.The Ti-Ce and Ti-La hybrid adsorbents obtained by the hydrolysis-precipitation method had much higher sorption capacity for fluoride than the TiO_(2) adsorbent prepared through hydrolysis.Rare earth(Ce and La)oxides and TiO_(2) exhibited a synergistic effect in the hybrid adsorbents for fluoride sorption.The sorption equilibrium of fluoride on the three adsorbents was achieved within 4 h,and the pseudo-second-order model described the sorption kinetics well.The sorption isotherms fitted the Langmuir model well,and the adsorption capacities of fluoride on the Ti-Ce and Ti-La adsorbents were about 9.6 and 15.1 mg·g^(-1),respectively,at the equilibrium fluoride concentration of 1.0 mg·L^(-1),much higher than the 1.7 mg·g^(-1) on the TiO_(2).The sorption capacities of fluoride on the three adsorbents decreased significantly when the solution pH increased from 3 to 9.5.The electrostatic interaction played an important role in fluoride removal by the three adsorbents,and Fourier transform infrared(FTIR)analysis indicated that the hydroxyl groups on the adsorbent surface were involved in fluoride adsorption.
基金supported by the National High Technology Research and Development of China(No.2013AA06A305)Program for Changjiang Scholars and Innovative Research Team in University,China Postdoctoral Science Foundation(2013T60128)Hundreds Talents Program of Chinese Academy of Sciences.
文摘Ozonation has been proved to be a promising approach for eliminating emerging pollutants in wastewater.In previous studies,emerging pollutants including diverse pharmaceuticals were found to exhibit significantly different ozonation reactivity.However,how the structural differences of emerging pollutants determine ozonation reactivity and mechanisms are still ambiguous.In this work,ozonation of dimethylaminophenazone(DMP)and acetylaminophenazone(AAA)with the same parent structure of phenazone but different substitution groups was investigated,in order to probe influencing mechanisms of structural differences on ozonation reactivity.Results show that DMP reacts with ozone and HOalmost 2 and 1 order of magnitude faster than AAA,respectively.At pH 8,HO· accelerates ozonation of DMP,but decreases ozonation of AAA.Competition simultaneously decreases degradation rate of the two phenazones,but effects on AAA are more significant than that on DMP.According to theoretical calculation results,differences in ozonation reactivity and mechanisms of the two phenazones can be mainly attributed to different substitution groups.The dimethylamino group in the structure of DMP increases the ozonation reactivity of phenazone by increasing reaction orbital energies and altering reaction sites,while the acetylamino group in the structure of AAA decreases the reaction orbital energy and therefore lowers the reactivity.
