Heavy metal(loid)s(HMs)pollution has become a common and complex problem in industrial parks due to rapid industrialization and urbanization.Here,soil and groundwater were sampled from a retired industrial park to inv...Heavy metal(loid)s(HMs)pollution has become a common and complex problem in industrial parks due to rapid industrialization and urbanization.Here,soil and groundwater were sampled from a retired industrial park to investigate the pollution characteristics of HMs.Results show that Ni,Pb,Cr,Zn,Cd,and Cu were the typical HMs in the soil.Source analysis with the positive matrix factorization model indicates that HMs in the topsoil stemmed from industrial activities,traffic emission,and natural source,and the groundwater HMs originated from industrial activities,groundwater-soil interaction,groundwater-rock interaction,and atmosphere deposition.The sequential extraction of soil HMs reveals that As and Hg were mainly distributed in the residue fraction,while Ni,Pb,Cr,Zn,Cd,and Cu mainly existed in the mobile fraction.Most HMs either in the total concentration or in the bioavailable fraction preferred to retain in soil as indicated by their high soil-water partitioning coefficients(K_(d)),and the K_(d) values were correlated with soil pH,groundwater redox potential,and dissolved oxygen.The relative stable soil-groundwater circumstance and the low active fraction contents limited the vertical migration of soil HMs and their release to groundwater.These findings increase our knowledge about HMs pollution characteristics of traditional industrial parks and provide a protocol for HMs pollution scrutinizing in large zones.展开更多
Disrupting effects of pollutants on symbiotic microbiota have been regarded as an important mechanism of host toxicity,with most current research focusing on the intestinal microbiota.In fact,the epidermal microbiota,...Disrupting effects of pollutants on symbiotic microbiota have been regarded as an important mechanism of host toxicity,with most current research focusing on the intestinal microbiota.In fact,the epidermal microbiota,which participates in the nutrient exchange between hosts and environments,could play a crucial role in host toxicity via community changes.To compare the contributions of intestinal and epidermal symbiotic microorganisms to host toxicity,this study designed single and combined scenarios of soil contamination[nano zerovalent iron(nZVI)and tris(2-chloroethyl)phosphate(TCEP)],and revealed the coupling mechanisms between intestinal/epidermal symbiotic bacterial communities and earthworm toxicological endpoints.Microbiome analysis showed that 15%of intestinal microbes were highly correlated with host endpoints,compared to 45%of epidermal microbes showing a similar correlation.Functional comparisons revealed that key species on the epidermis were mainly heterotrophic microbes with genetic abilities to utilize metal elements and carbohydrate nutrients.Further verifications demonstrated that when facing the co-contamination of nZVI and TCEP,certain symbiotic microorganisms became dominant and consumed zinc,copper,and manganese along with saccharides and amino acids,which may be responsible for the nutritional deficiencies in the host earthworms.The findings can enrich the understanding of the coupling relationship between symbiotic microorganisms and host toxicity,highlighting the importance of epidermal microorganisms in host resistance to environmental pollution.展开更多
Polychlorinated biphenyls(PCBs)with different chlorine substitution patterns often coexist in e-waste-processing sites.However,the single and combined toxicity of PCBs to soil organisms and the influence of chlorine s...Polychlorinated biphenyls(PCBs)with different chlorine substitution patterns often coexist in e-waste-processing sites.However,the single and combined toxicity of PCBs to soil organisms and the influence of chlorine substitution patterns remain largely unknown.Herein,we evaluated the distinct in vivo toxicity of PCB28(a trichlorinated PCB),PCB52(a tetrachlorinated PCB),PCB101(a pentachlorinated PCB),and their mixture to earthworm Eisenia fetida in soil,and looked into the underlining mechanisms in an in vitro test using coelomocytes.After a 28-days exposure,all PCBs(up to 10 mg/kg)were not fatal to earthworms,but could induce intestinal histopathological changes and microbial community alterations in the drilosphere system,along with a significant weight loss.Notably,pentachlorinated PCBs with a low bioaccumulation ability showed greater inhibitory effects on the growth of earthworm than lowly chlorinated PCBs,suggesting that bioaccumulation was not the main determinant of chlorine substitution-dependent toxicity.Furthermore,in vitro assays showed that the highly chlorinated PCBs induced a high-percentage apoptosis of eleocytes in the coelomocytes and significantly activated antioxidant enzymes,indicating that the distinct cellular vulnerability to lowly/highly chlorinated PCBs was the main contributor to the PCBs toxicity.These findings emphasize the specific advantage of using earthworms in the control of lowly chlorinated PCBs in soil due to their high tolerance and accumulation ability.展开更多
The overall cross-media risk evaluation of organic pollutants in retired industrial parks is insufficiently recognized.In this study,11 semi-volatile organic compounds(SVOCs)and 27 volatile organic compounds(VOCs)were...The overall cross-media risk evaluation of organic pollutants in retired industrial parks is insufficiently recognized.In this study,11 semi-volatile organic compounds(SVOCs)and 27 volatile organic compounds(VOCs)were measured in 531 soil and groundwater samples taken from a retired industrial park by coast in Zhejiang Province,China.Total petroleum hydrocarbons(TPHs),Di(2-ethylhexyl)phthalate(DEHP),benzene,and ethylbenzene were identified as the critical pollutants in the soil,while TPHs,1,2-dichloropropane(1,2-DCP),toluene,benzo[a]anthracene(BaA),and benzo[b]fluoranthene(BbF)were identified as critical pollutants in the groundwater for exceeding China national standards.The spatial correlation between the concentrations of organic pollutants in soil and groundwater was explored by employing the Geodetector model.Based on the results of spatial interpolation,high-risk hotspots regarding soil and groundwater pollution were identified.Moreover,the possible harm to human health of the critical pollutants were also under evaluation.Among various critical pollutants,benzene,ethylbenzene,and DEHP in soil,and 1,2-DCP in groundwater,were the main contributors to the overall health risk of multimedia pollution.This study developed a comprehensive approach to assess the risks posed by specific organic toxicants in various environmental media.The findings of this work can serve as a valuable reference for future management strategies in retired industrial parks.展开更多
Nonradical oxidation based on peroxydisulfate(PDS)activation has attracted increasing attention for selective degradation of organic pollutants.Herein,topological defects were introduced into biochar(BC)via removing N...Nonradical oxidation based on peroxydisulfate(PDS)activation has attracted increasing attention for selective degradation of organic pollutants.Herein,topological defects were introduced into biochar(BC)via removing N atoms in N-doped BC(NBC)in an attempt to improve the nonradical catalytic performance.Compared to the pristine BC and NBC,the introduction of topological defects could achieve up to 36.6-and 8.7-times catalytic activity enhancement,respectively.More importantly,it was found that the catalytic activity was dominated by topological defects,which was verified by the significant positive correlation between the pseudo-first-order rate constants and the content of topological defects.Theoretical calculations suggested that topological defects enhanced the electrondonating ability of BC by reducing the energy gap,which made the electrons transfer to PDS molecules more easily.As a result,holes were generated after the carbon defects lost electrons,and induced a nonradical oxidation process.Benefiting from the merits of nonradical oxidation,the developed BC/PDS system showed superior performance in removing electron-rich contaminants in the presence of inorganic anions and in the actual environments.This study not only provides a potential avenue for designing efficient biochar-based catalysts,but also advances the mechanism understanding of nonradical oxidation process induced by carbon defects.展开更多
1Introduction Due to the easy loss and decomposition of traditional chemical pesticides,their repeated application in agriculture results in serious environmental risks to the surrounding environment and organisms.Con...1Introduction Due to the easy loss and decomposition of traditional chemical pesticides,their repeated application in agriculture results in serious environmental risks to the surrounding environment and organisms.Controlledrelease nanopesticides are attracting attention as a promising technology in agriculture due to their unique structure and effects(e.g.,nano-size scale,interfacial effects,and effective insecticidal time)(An et al.,2022).Their application could improve insecticidal efficacies,decrease usage amounts,and reduce the potential environmental impacts of chemical pesticides.展开更多
Coagulation followed by sedimentation, as a conventional technique in the water treatment plant, can be the first line of defense against exposures of carbon nanotubes （CNTs） to aquatic organisms and human beings, w...Coagulation followed by sedimentation, as a conventional technique in the water treatment plant, can be the first line of defense against exposures of carbon nanotubes （CNTs） to aquatic organisms and human beings, which has been rarely documented. This study investigated the removal of dispersant-stabilized CNT suspensions by poly aluminum chloride （PAC1） and KAl（SO4）2-12H20 （alum）, with a focus on the effects of dispersant type, coagulant type and dosage. PAC1 performed better than alum in the removal of tannic acid-, humic acid-, and sodium dodecyl benzenesulfonate-stabilized CNTs, but worse for polyethylene glycol octylphenyl ether （TX100）-stabilized CNTs. Neither coagulant could effectively precipitate cetyltrimethyl ammonium bromide-stabilized CNTs. The removal by PACl first increased up to a plateau and then decreased with the continued increase of coagulant dosage. However, the removal rates leveled off but did not decrease after achieving their highest level with the continued addition of alum. The coagulation and flocculation of the CNT suspensions by PACl could be regulated mainly by the mechanism of adsorption charge neutralization, whereas the coagulation by alum mainly involved electrical double-layer compression.展开更多
Sorption kinetics of organic compounds on biochars is important for understanding the retardation of mobility and bioavailability of organic compounds.Herein,sorption kinetics of 1,3,5-trinitrobenzene on biochars prep...Sorption kinetics of organic compounds on biochars is important for understanding the retardation of mobility and bioavailability of organic compounds.Herein,sorption kinetics of 1,3,5-trinitrobenzene on biochars prepared from 200 to 700℃was investigated to explore the sorption process.Loose partition matrix and condensed partition matrix were formed at relatively low and moderate temperatures,respectively.However,biochars produced at relatively high temperatures formed rich pore structures.Therefore,sorption equilibrium time of 1,3,5-trinitrobenzene increased with increasing preparation temperature from 200 to 350℃due to the slower diffusion rate in the more condensed matrix,and then decreased when preparation temperature was higher than 400℃because of the faster adsorption rate in the greater number of pores.Linear positive relationship between matrix diffusion rates of 1,3,5-trinitrobenzene on biochars prepared at 200,250,300,350℃and H/C ratios of biochars was observed,suggesting that the inhibition of partition process was caused by the condensed matrix in biochars.Linear positive relationships between adsorption rates(i.e.,fast outer diffusion rate and slow pore diffusion rate)of 1,3,5-trinitrobenzene on biochars prepared at 400,450,550,700℃and graphite defects of biochars were observed,because the increase of graphite defects of biochars could promote the adsorption by increasing the quantity of fast diffusion channels and sorption sites.This study reveals the underlying mechanisms of sorption kinetics for organic compounds with relatively large size on biochars,which has potential guidance for the application of biochars and prediction of the environmental risks of organic compounds.展开更多
With the fast development of nanotechnology,reactive engineered nanomaterials(ENMs)are increasingly discharged into the environment,where they interact with environmental components and organisms and thus pose potenti...With the fast development of nanotechnology,reactive engineered nanomaterials(ENMs)are increasingly discharged into the environment,where they interact with environmental components and organisms and thus pose potential risks.The interactions-derived formation of nano-environmental and nano-bio interfaces determines environmental behaviors and biological effects of ENMs,and ubiquitous dissolved organic matter(DOM)is bound to impact the interfacial interactions and the resulted environmental risks.Herein,we systematically investigated adsorptive interactions between ENMs and various DOM representatives,and thereby demonstrated the effects of DOM on the aqueous suspension/aggregation,mobility in porous media,adsorption of contaminants,transformation,and biological accumulation and toxicity of ENMs.Overall,we conclude that natural DOM can in general expand environmental distribution of ENMs while limit their toxicity to organisms.展开更多
Since the beginning of the 21 st century,the increasing production and application of nano-TiO_(2)in consumer products have inevitably led to its release into aquatic systems and therefore caused the exposure of aquat...Since the beginning of the 21 st century,the increasing production and application of nano-TiO_(2)in consumer products have inevitably led to its release into aquatic systems and therefore caused the exposure of aquatic organisms,resulting in growing environmental concerns.However,the safety of nano-TiO_(2)in aquatic environments has not been systematically assessed,especially in coastal and estuary waters where a large number of filterfeeding animals live.Bivalves are considered around the world to be a unique target group for nanoparticle toxicity,and numerous studies have been conducted to test the toxic effects of nano-TiO_(2)on bivalves.The aim of this review was to systematically summarize and analyze published data concerning the toxicological effects of nano-TiO_(2)in bivalves.In particular,the toxicity of nano-TiO_(2)to the antioxidant system and cell physiology was subjected to meta-analysis to reveal the mechanism of the toxicological effects of nano-TiO_(2)and the factors affecting its toxicological effects.To reveal the cooperation,hot keywords and cocitations in this field,bibliometric analysis was conducted,and the results showed that the toxicological molecular mechanisms of nano-TiO_(2)and the combined effects of nano-TiO_(2)and other environmental factors are two major hot spots.Finally,some perspectives and insights were provided in this review for future research on nano-TiO_(2)toxicology in bivalves.展开更多
Surface oxidation can alter physicochemical properties of multiwalled carbon nanotubes(MWCNTs) and influence their aqueous stabilization.Many techniques have been used to characterize the physicochemical properties an...Surface oxidation can alter physicochemical properties of multiwalled carbon nanotubes(MWCNTs) and influence their aqueous stabilization.Many techniques have been used to characterize the physicochemical properties and aqueous stabilization of MWCNTs.However,the relationship between the change in physicochemical property and the aqueous stabilization of MWCNTs merits more studies,and the multiple characterization techniques have not been well compared.This study systematically and comparatively investigated the effect of oxidation on the physicochemical properties and aqueous stabilization of MWCNTs using multiple analysis methods.Increased surface area,disclosed tube ends,defects on the sidewalls,disruption of the electronic structure,and removal of metal catalysts and amorphous carbon were observed for the oxidized MWCNTs(o-MWCNTs) using the multipoint Brunauer-Emmett-Teller(BET) method,transmission electron microscope observation,Raman spectroscopy,UV-Vis spectroscopy,and thermogravimetric analysis.An oxidation-time-dependent increase in oxygen content of the MWCNTs was verified by the methods of elemental analysis,mass difference calculation,and X-ray photoelectron spectroscopy(XPS).Fourier transform infrared spectroscopy,XPS,and the Boehm titration were employed to study the functionalities on the MWCNT surfaces.Despite the limitations of these techniques,the results indicated that the dramatic increase in carboxyl groups was mainly responsible for the significant increase in oxygen content after the oxidation.The dissociation of the grafted functional groups increased electronegativity of the o-MWCNTs and facilitated the aqueous stabilization of o-MWCNTs through electrostatic repulsions.The oxidation affected the UV-Vis absorbance of MWCNT suspensions.The absorbances at 800 nm of the stabilized MWCNT suspensions had a good correlation with the MWCNT concentrations and could be used to quantify the MWCNT suspensions.The findings of this work are expected to boost the research on carbon nanotubes and their environmental behaviors.展开更多
The release of biochar colloids considerably affects the stability of biochar in environment.Currently,information on the release behavior and suspension stability of biochar colloids in real soil solutions is scarce....The release of biochar colloids considerably affects the stability of biochar in environment.Currently,information on the release behavior and suspension stability of biochar colloids in real soil solutions is scarce.In this study,20 soils were collected from different districts in China and the release behavior of biochar colloids and their suspension stability in soil solutions were systematically examined.The results showed that both pyrolysis temperature and biomass source had important effects on the formation of biochar colloids in soil solutions.The formation amount of biochar colloids from low pyrolysis temperatures(400℃)(average amount of 9.33-16.41 mg/g)were significantly higher than those from high pyrolysis temperatures(700℃)(average amount of less than 2 mg/g).The formation amount of wheat straw-derived biochar colloids were higher than those of rice straw-derived biochar colloids probably due to the higher O/C ratio in wheat-straw biochar.Further,biochar colloidal formation amount was negatively correlated with comprehensive effect of dissolved organic carbon,Fe and Al in soil solutions.The sedimentation curve of biochar colloids in soil solutions is well described by an exponential model and demonstrated high suspension stability.Around 40%of the biochar colloids were maintained in the suspension at the final sedimentation equilibrium.The settling efficiency of biochar colloids was positively correlated with comprehensive effect of the ionic strength and K,Ca,Na,and Mg contents in soil solutions.Our findings help promote a deeper understanding of biochar loss and stability in the soil-water environment.展开更多
With increasing environmental application,biochar(BC)will inevitably interact with and impact environmental behaviors of widely distributed extracellular DNA(eDNA),which however still remains to be studied.Herein,the ...With increasing environmental application,biochar(BC)will inevitably interact with and impact environmental behaviors of widely distributed extracellular DNA(eDNA),which however still remains to be studied.Herein,the adsorption/desorption and the degradation by nucleases of eDNA on three aromatized BCs pyrolyzed at 700℃were firstly investigated.The results show that the eDNA was irreversibly adsorbed by aromatized BCs and the pseudo-second-order and Freundlich models accurately described the adsorption process.Increasing solution ionic strength or decreasing pH below 5.0 significantly increased the eDNA adsorption on BCs.However,increasing pH from 5.0 to 10.0 faintly decreased eDNA adsorption.Electrostatic interaction,Ca ion bridge interaction,andπ-πinteraction between eDNA and BC could dominate the eDNA adsorption,while ligand exchange and hydrophobic interactions were minor contributors.The presence of BCs provided a certain protection to eDNA against degradation by DNase I.BC-bound eDNA could be partly degraded by nuclease,while BC-bound nuclease completely lost its degradability.These findings are of fundamental significance for the potential application of biochar in eDNA dissemination management and evaluating the environmental fate of eDNA.展开更多
The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability a...The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability and risks of HOCs in the environment.In previous study,inspired from the competitive adsorption on activated carbon(AC),the displaceable fraction of HOCs sorption to soot by competitor was attributed to the adsorption on elemental carbon fraction of soot(EC-Soot),while the linear and nondisplaceable fraction was attributed to the partition in authigenic organic matter of soot(OM-Soot).In this study,however,we observed that the linear and nondisplaceable fraction of HOC(naphthalene)to a diesel soot(D-Soot)by competitor(phenanthrene or p-nitrophenol)should be attributed to not only the linear partition in OM-Soot,but also the residual linear adsorption on EC-Soot.We also observed that the competition on the surface of soot dominated by external surface was different from that of AC dominated by micropore surface,i.e.,complete displacement of HOCs by p-nitrophenol could occur for the micropore surface of AC,but not for the external surface of soot.These observations were obtained through the separation of EC-Soot and OM-Soot from D-Soot with organic-solvent extraction and the sorption comparisons of D-Soot with an AC(ACF300)and a multiwalled carbon nanotube(MWCNT30).The obtained results would give new insights to the sorption mechanisms of HOCs by soot and help to assess their environmental risks.展开更多
基金supported by the Science and Technology Research Program of Zhejiang Province(No.2020C03011)the National Key Research and Development Program of China(No.2022YFC3702100)Zhejiang Provincial Natural Science Foundation of China(No.LD21B070001)。
文摘Heavy metal(loid)s(HMs)pollution has become a common and complex problem in industrial parks due to rapid industrialization and urbanization.Here,soil and groundwater were sampled from a retired industrial park to investigate the pollution characteristics of HMs.Results show that Ni,Pb,Cr,Zn,Cd,and Cu were the typical HMs in the soil.Source analysis with the positive matrix factorization model indicates that HMs in the topsoil stemmed from industrial activities,traffic emission,and natural source,and the groundwater HMs originated from industrial activities,groundwater-soil interaction,groundwater-rock interaction,and atmosphere deposition.The sequential extraction of soil HMs reveals that As and Hg were mainly distributed in the residue fraction,while Ni,Pb,Cr,Zn,Cd,and Cu mainly existed in the mobile fraction.Most HMs either in the total concentration or in the bioavailable fraction preferred to retain in soil as indicated by their high soil-water partitioning coefficients(K_(d)),and the K_(d) values were correlated with soil pH,groundwater redox potential,and dissolved oxygen.The relative stable soil-groundwater circumstance and the low active fraction contents limited the vertical migration of soil HMs and their release to groundwater.These findings increase our knowledge about HMs pollution characteristics of traditional industrial parks and provide a protocol for HMs pollution scrutinizing in large zones.
基金supported by the National Key Research and Development Program of China(2022YFC3702103)the Natural Science Foundation of China(U21A20163,42192573,22376181)the Zhejiang Provincial Natural Science Foundation of China(LD21B070001).
文摘Disrupting effects of pollutants on symbiotic microbiota have been regarded as an important mechanism of host toxicity,with most current research focusing on the intestinal microbiota.In fact,the epidermal microbiota,which participates in the nutrient exchange between hosts and environments,could play a crucial role in host toxicity via community changes.To compare the contributions of intestinal and epidermal symbiotic microorganisms to host toxicity,this study designed single and combined scenarios of soil contamination[nano zerovalent iron(nZVI)and tris(2-chloroethyl)phosphate(TCEP)],and revealed the coupling mechanisms between intestinal/epidermal symbiotic bacterial communities and earthworm toxicological endpoints.Microbiome analysis showed that 15%of intestinal microbes were highly correlated with host endpoints,compared to 45%of epidermal microbes showing a similar correlation.Functional comparisons revealed that key species on the epidermis were mainly heterotrophic microbes with genetic abilities to utilize metal elements and carbohydrate nutrients.Further verifications demonstrated that when facing the co-contamination of nZVI and TCEP,certain symbiotic microorganisms became dominant and consumed zinc,copper,and manganese along with saccharides and amino acids,which may be responsible for the nutritional deficiencies in the host earthworms.The findings can enrich the understanding of the coupling relationship between symbiotic microorganisms and host toxicity,highlighting the importance of epidermal microorganisms in host resistance to environmental pollution.
基金This work was supported by the National Key Research and Development Program of China(No.2017YFA0207003)the National Natural Science Foundation of China(No.21777139).
文摘Polychlorinated biphenyls(PCBs)with different chlorine substitution patterns often coexist in e-waste-processing sites.However,the single and combined toxicity of PCBs to soil organisms and the influence of chlorine substitution patterns remain largely unknown.Herein,we evaluated the distinct in vivo toxicity of PCB28(a trichlorinated PCB),PCB52(a tetrachlorinated PCB),PCB101(a pentachlorinated PCB),and their mixture to earthworm Eisenia fetida in soil,and looked into the underlining mechanisms in an in vitro test using coelomocytes.After a 28-days exposure,all PCBs(up to 10 mg/kg)were not fatal to earthworms,but could induce intestinal histopathological changes and microbial community alterations in the drilosphere system,along with a significant weight loss.Notably,pentachlorinated PCBs with a low bioaccumulation ability showed greater inhibitory effects on the growth of earthworm than lowly chlorinated PCBs,suggesting that bioaccumulation was not the main determinant of chlorine substitution-dependent toxicity.Furthermore,in vitro assays showed that the highly chlorinated PCBs induced a high-percentage apoptosis of eleocytes in the coelomocytes and significantly activated antioxidant enzymes,indicating that the distinct cellular vulnerability to lowly/highly chlorinated PCBs was the main contributor to the PCBs toxicity.These findings emphasize the specific advantage of using earthworms in the control of lowly chlorinated PCBs in soil due to their high tolerance and accumulation ability.
基金supported by the Consulting Research Project of the Chinese Academy of Engineering(No.2023-XZ-37)the Science and Technology Research Program of Zhejiang Province(China)(No.2020C03011).
文摘The overall cross-media risk evaluation of organic pollutants in retired industrial parks is insufficiently recognized.In this study,11 semi-volatile organic compounds(SVOCs)and 27 volatile organic compounds(VOCs)were measured in 531 soil and groundwater samples taken from a retired industrial park by coast in Zhejiang Province,China.Total petroleum hydrocarbons(TPHs),Di(2-ethylhexyl)phthalate(DEHP),benzene,and ethylbenzene were identified as the critical pollutants in the soil,while TPHs,1,2-dichloropropane(1,2-DCP),toluene,benzo[a]anthracene(BaA),and benzo[b]fluoranthene(BbF)were identified as critical pollutants in the groundwater for exceeding China national standards.The spatial correlation between the concentrations of organic pollutants in soil and groundwater was explored by employing the Geodetector model.Based on the results of spatial interpolation,high-risk hotspots regarding soil and groundwater pollution were identified.Moreover,the possible harm to human health of the critical pollutants were also under evaluation.Among various critical pollutants,benzene,ethylbenzene,and DEHP in soil,and 1,2-DCP in groundwater,were the main contributors to the overall health risk of multimedia pollution.This study developed a comprehensive approach to assess the risks posed by specific organic toxicants in various environmental media.The findings of this work can serve as a valuable reference for future management strategies in retired industrial parks.
基金National Key Research and Development Program of China(2021YFC1809204)National Natural Science Foundation of China(42192573,21621005,and U21A20163)+1 种基金Research and Development Program of Zhejiang Province,China(2021C0167)Fundamental Research Funds for the Central Universities(226-2022-00212).
文摘Nonradical oxidation based on peroxydisulfate(PDS)activation has attracted increasing attention for selective degradation of organic pollutants.Herein,topological defects were introduced into biochar(BC)via removing N atoms in N-doped BC(NBC)in an attempt to improve the nonradical catalytic performance.Compared to the pristine BC and NBC,the introduction of topological defects could achieve up to 36.6-and 8.7-times catalytic activity enhancement,respectively.More importantly,it was found that the catalytic activity was dominated by topological defects,which was verified by the significant positive correlation between the pseudo-first-order rate constants and the content of topological defects.Theoretical calculations suggested that topological defects enhanced the electrondonating ability of BC by reducing the energy gap,which made the electrons transfer to PDS molecules more easily.As a result,holes were generated after the carbon defects lost electrons,and induced a nonradical oxidation process.Benefiting from the merits of nonradical oxidation,the developed BC/PDS system showed superior performance in removing electron-rich contaminants in the presence of inorganic anions and in the actual environments.This study not only provides a potential avenue for designing efficient biochar-based catalysts,but also advances the mechanism understanding of nonradical oxidation process induced by carbon defects.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(No.LD21B070001)。
文摘1Introduction Due to the easy loss and decomposition of traditional chemical pesticides,their repeated application in agriculture results in serious environmental risks to the surrounding environment and organisms.Controlledrelease nanopesticides are attracting attention as a promising technology in agriculture due to their unique structure and effects(e.g.,nano-size scale,interfacial effects,and effective insecticidal time)(An et al.,2022).Their application could improve insecticidal efficacies,decrease usage amounts,and reduce the potential environmental impacts of chemical pesticides.
基金supported by the National Basic Research Program (973) of China (No. 2008CB418204)the National Natural Science Foundation of China (No. 21077089,40873072)+1 种基金the Zhejiang Provincial "Qianjiang Talent Program" (No. 2010R10041)Zhejiang Provincial Innovative Research Team of Water Treatment Functional Materials and their Application
文摘Coagulation followed by sedimentation, as a conventional technique in the water treatment plant, can be the first line of defense against exposures of carbon nanotubes （CNTs） to aquatic organisms and human beings, which has been rarely documented. This study investigated the removal of dispersant-stabilized CNT suspensions by poly aluminum chloride （PAC1） and KAl（SO4）2-12H20 （alum）, with a focus on the effects of dispersant type, coagulant type and dosage. PAC1 performed better than alum in the removal of tannic acid-, humic acid-, and sodium dodecyl benzenesulfonate-stabilized CNTs, but worse for polyethylene glycol octylphenyl ether （TX100）-stabilized CNTs. Neither coagulant could effectively precipitate cetyltrimethyl ammonium bromide-stabilized CNTs. The removal by PACl first increased up to a plateau and then decreased with the continued increase of coagulant dosage. However, the removal rates leveled off but did not decrease after achieving their highest level with the continued addition of alum. The coagulation and flocculation of the CNT suspensions by PACl could be regulated mainly by the mechanism of adsorption charge neutralization, whereas the coagulation by alum mainly involved electrical double-layer compression.
基金the National Key Research and Development Program of China(2021YFC1809204 and 2017YFA0207001)the National Natural Science Foundation of China(21777138)the Key Research and Development Program of Zhejiang Province,China(2020C03011 and 2021C03167).
文摘Sorption kinetics of organic compounds on biochars is important for understanding the retardation of mobility and bioavailability of organic compounds.Herein,sorption kinetics of 1,3,5-trinitrobenzene on biochars prepared from 200 to 700℃was investigated to explore the sorption process.Loose partition matrix and condensed partition matrix were formed at relatively low and moderate temperatures,respectively.However,biochars produced at relatively high temperatures formed rich pore structures.Therefore,sorption equilibrium time of 1,3,5-trinitrobenzene increased with increasing preparation temperature from 200 to 350℃due to the slower diffusion rate in the more condensed matrix,and then decreased when preparation temperature was higher than 400℃because of the faster adsorption rate in the greater number of pores.Linear positive relationship between matrix diffusion rates of 1,3,5-trinitrobenzene on biochars prepared at 200,250,300,350℃and H/C ratios of biochars was observed,suggesting that the inhibition of partition process was caused by the condensed matrix in biochars.Linear positive relationships between adsorption rates(i.e.,fast outer diffusion rate and slow pore diffusion rate)of 1,3,5-trinitrobenzene on biochars prepared at 400,450,550,700℃and graphite defects of biochars were observed,because the increase of graphite defects of biochars could promote the adsorption by increasing the quantity of fast diffusion channels and sorption sites.This study reveals the underlying mechanisms of sorption kinetics for organic compounds with relatively large size on biochars,which has potential guidance for the application of biochars and prediction of the environmental risks of organic compounds.
基金This work was supported by the National Key Research and Development Program of China(2017YFA0207003)the National Natural Science Foundation of China(21525728 and 21621005).
文摘With the fast development of nanotechnology,reactive engineered nanomaterials(ENMs)are increasingly discharged into the environment,where they interact with environmental components and organisms and thus pose potential risks.The interactions-derived formation of nano-environmental and nano-bio interfaces determines environmental behaviors and biological effects of ENMs,and ubiquitous dissolved organic matter(DOM)is bound to impact the interfacial interactions and the resulted environmental risks.Herein,we systematically investigated adsorptive interactions between ENMs and various DOM representatives,and thereby demonstrated the effects of DOM on the aqueous suspension/aggregation,mobility in porous media,adsorption of contaminants,transformation,and biological accumulation and toxicity of ENMs.Overall,we conclude that natural DOM can in general expand environmental distribution of ENMs while limit their toxicity to organisms.
基金supported by the Natural Science Foundation of China(No.31872587)the Shanghai Pujiang Talent Program(No.18PJ1404000)+1 种基金Shanghai Municipal Natural Science Foundation(No.17ZR1412900)the National Key Research and Development Program of China(No.2017YFA0207003)。
文摘Since the beginning of the 21 st century,the increasing production and application of nano-TiO_(2)in consumer products have inevitably led to its release into aquatic systems and therefore caused the exposure of aquatic organisms,resulting in growing environmental concerns.However,the safety of nano-TiO_(2)in aquatic environments has not been systematically assessed,especially in coastal and estuary waters where a large number of filterfeeding animals live.Bivalves are considered around the world to be a unique target group for nanoparticle toxicity,and numerous studies have been conducted to test the toxic effects of nano-TiO_(2)on bivalves.The aim of this review was to systematically summarize and analyze published data concerning the toxicological effects of nano-TiO_(2)in bivalves.In particular,the toxicity of nano-TiO_(2)to the antioxidant system and cell physiology was subjected to meta-analysis to reveal the mechanism of the toxicological effects of nano-TiO_(2)and the factors affecting its toxicological effects.To reveal the cooperation,hot keywords and cocitations in this field,bibliometric analysis was conducted,and the results showed that the toxicological molecular mechanisms of nano-TiO_(2)and the combined effects of nano-TiO_(2)and other environmental factors are two major hot spots.Finally,some perspectives and insights were provided in this review for future research on nano-TiO_(2)toxicology in bivalves.
基金supported by the National Natural Science Foundation of China(21525728,21337004,21477107)the National Basic Research Program of China(2014CB441104)the Specialized Research Fund for the Doctoral Program of Higher Education (20130101110132)
文摘Surface oxidation can alter physicochemical properties of multiwalled carbon nanotubes(MWCNTs) and influence their aqueous stabilization.Many techniques have been used to characterize the physicochemical properties and aqueous stabilization of MWCNTs.However,the relationship between the change in physicochemical property and the aqueous stabilization of MWCNTs merits more studies,and the multiple characterization techniques have not been well compared.This study systematically and comparatively investigated the effect of oxidation on the physicochemical properties and aqueous stabilization of MWCNTs using multiple analysis methods.Increased surface area,disclosed tube ends,defects on the sidewalls,disruption of the electronic structure,and removal of metal catalysts and amorphous carbon were observed for the oxidized MWCNTs(o-MWCNTs) using the multipoint Brunauer-Emmett-Teller(BET) method,transmission electron microscope observation,Raman spectroscopy,UV-Vis spectroscopy,and thermogravimetric analysis.An oxidation-time-dependent increase in oxygen content of the MWCNTs was verified by the methods of elemental analysis,mass difference calculation,and X-ray photoelectron spectroscopy(XPS).Fourier transform infrared spectroscopy,XPS,and the Boehm titration were employed to study the functionalities on the MWCNT surfaces.Despite the limitations of these techniques,the results indicated that the dramatic increase in carboxyl groups was mainly responsible for the significant increase in oxygen content after the oxidation.The dissociation of the grafted functional groups increased electronegativity of the o-MWCNTs and facilitated the aqueous stabilization of o-MWCNTs through electrostatic repulsions.The oxidation affected the UV-Vis absorbance of MWCNT suspensions.The absorbances at 800 nm of the stabilized MWCNT suspensions had a good correlation with the MWCNT concentrations and could be used to quantify the MWCNT suspensions.The findings of this work are expected to boost the research on carbon nanotubes and their environmental behaviors.
基金the National Natural Science Foundation of China(Nos.21976158 and 21677129)。
文摘The release of biochar colloids considerably affects the stability of biochar in environment.Currently,information on the release behavior and suspension stability of biochar colloids in real soil solutions is scarce.In this study,20 soils were collected from different districts in China and the release behavior of biochar colloids and their suspension stability in soil solutions were systematically examined.The results showed that both pyrolysis temperature and biomass source had important effects on the formation of biochar colloids in soil solutions.The formation amount of biochar colloids from low pyrolysis temperatures(400℃)(average amount of 9.33-16.41 mg/g)were significantly higher than those from high pyrolysis temperatures(700℃)(average amount of less than 2 mg/g).The formation amount of wheat straw-derived biochar colloids were higher than those of rice straw-derived biochar colloids probably due to the higher O/C ratio in wheat-straw biochar.Further,biochar colloidal formation amount was negatively correlated with comprehensive effect of dissolved organic carbon,Fe and Al in soil solutions.The sedimentation curve of biochar colloids in soil solutions is well described by an exponential model and demonstrated high suspension stability.Around 40%of the biochar colloids were maintained in the suspension at the final sedimentation equilibrium.The settling efficiency of biochar colloids was positively correlated with comprehensive effect of the ionic strength and K,Ca,Na,and Mg contents in soil solutions.Our findings help promote a deeper understanding of biochar loss and stability in the soil-water environment.
基金supported by the National Natural Science Foundation of China(Nos.21976158,21525728,and 21677129)。
文摘With increasing environmental application,biochar(BC)will inevitably interact with and impact environmental behaviors of widely distributed extracellular DNA(eDNA),which however still remains to be studied.Herein,the adsorption/desorption and the degradation by nucleases of eDNA on three aromatized BCs pyrolyzed at 700℃were firstly investigated.The results show that the eDNA was irreversibly adsorbed by aromatized BCs and the pseudo-second-order and Freundlich models accurately described the adsorption process.Increasing solution ionic strength or decreasing pH below 5.0 significantly increased the eDNA adsorption on BCs.However,increasing pH from 5.0 to 10.0 faintly decreased eDNA adsorption.Electrostatic interaction,Ca ion bridge interaction,andπ-πinteraction between eDNA and BC could dominate the eDNA adsorption,while ligand exchange and hydrophobic interactions were minor contributors.The presence of BCs provided a certain protection to eDNA against degradation by DNase I.BC-bound eDNA could be partly degraded by nuclease,while BC-bound nuclease completely lost its degradability.These findings are of fundamental significance for the potential application of biochar in eDNA dissemination management and evaluating the environmental fate of eDNA.
基金supported partly by the National Natural Science Foundation of China(Nos.21777138 and 21621005)the National Key Research and Development Program of China(No.2017YFA0207001)+1 种基金the Key Research and Development Program of Zhejiang Province(No.2019C03105)。
文摘The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability and risks of HOCs in the environment.In previous study,inspired from the competitive adsorption on activated carbon(AC),the displaceable fraction of HOCs sorption to soot by competitor was attributed to the adsorption on elemental carbon fraction of soot(EC-Soot),while the linear and nondisplaceable fraction was attributed to the partition in authigenic organic matter of soot(OM-Soot).In this study,however,we observed that the linear and nondisplaceable fraction of HOC(naphthalene)to a diesel soot(D-Soot)by competitor(phenanthrene or p-nitrophenol)should be attributed to not only the linear partition in OM-Soot,but also the residual linear adsorption on EC-Soot.We also observed that the competition on the surface of soot dominated by external surface was different from that of AC dominated by micropore surface,i.e.,complete displacement of HOCs by p-nitrophenol could occur for the micropore surface of AC,but not for the external surface of soot.These observations were obtained through the separation of EC-Soot and OM-Soot from D-Soot with organic-solvent extraction and the sorption comparisons of D-Soot with an AC(ACF300)and a multiwalled carbon nanotube(MWCNT30).The obtained results would give new insights to the sorption mechanisms of HOCs by soot and help to assess their environmental risks.
