The concentration and composition of nutrients,such as N,P,and Si,respond to biogeochemical processes and in turn,impact the phytoplanktons'community structure and primary production.In this study,historical data ...The concentration and composition of nutrients,such as N,P,and Si,respond to biogeochemical processes and in turn,impact the phytoplanktons'community structure and primary production.In this study,historical data was systematically analyzed to identify long-term variations in nutrient trends,red tide frequency,phytoplankton community abundance,and dominant species succession in the southern Yellow Sea(SYS).Results showed that N/P concentration ratios dramatically increased as a function of increasing dissolved inorganic nitrogen concentrations,and Si/N concentration ratios were generally larger than 1,indicating that N limitation morphed to P limitation and potentially to Si limitation,which impacted the phytoplankton community.Furthermore,inter-annual trends over the past 50 years show that phytoplankton community abundance has been higher in spring and summer,relative to autumn and winter.Moreover,with respect to red tide frequency,diatom abundance gradually decreased,while that of dinoflagellates gradually increased.Dominant species succession showed that the phytoplankton community exhibited an evident tendency to transform from diatoms to dinoflagellates.These research results clearly depict the presence of an important correlation between the phytoplankton community and nutrient structure in the SYS.展开更多
Parent and alkylated polycyclic aromatic hydrocarbons(alkyl-PAHs),which are a class of important toxic components of crude oil especially in the marine environment,exhibit adverse effects on aquatic life and potential...Parent and alkylated polycyclic aromatic hydrocarbons(alkyl-PAHs),which are a class of important toxic components of crude oil especially in the marine environment,exhibit adverse effects on aquatic life and potentially pose a human health risk.However,the lack of chronic toxicity data is one of the hindrances for alkylPAHs when assessing their ecological risks.In this study,predicted no-effect concentrations(PNECs)in seawater and marine sediment for ten parent-and alkyl-PAHs were derived by applying species sensitivity distributions(SSDs)and quantitative structure-activity relationships(QSARs).The local area,Dalian Bay,where an oil-spilled accident happened in 2010,was chosen as a case site to assess ecological risks for ten PAHs in surface seawaters and marine sediments.Their PNECs in seawater and sediment for protecting aquatic organisms in marine ecosystems were calculated and recommended in the range of 0.012-2.79μg/L and 48.2-1337 ng/g(dry weight),respectively.Overall,the derived PNECs for the studied PAHs in seawater and marine sediment were comparable to those obtained by classical methods.Risk quotient results indicate low ecological risks to ecosystems for ten parent-and alkyl-PAHs in surface seawaters and surface sediments from the Dalian Bay.These findings provide a first insight into the PNECs and ecological risks of alkyl-PAHs,emphasizing the role of the computational toxicology in ecological risk assessments.The use of QSARs has been identified as a valuable tool for preliminarily assessing ecological risks of emerging pollutants,being more predictable of real exposure scenarios for risk assessment purposes.展开更多
Environmental pollution from synthetic chemical mixtures has significant adverse impacts on marine ecosystems.However,identifying the main constituents of chemical mixtures that pose ecological threats is challenging ...Environmental pollution from synthetic chemical mixtures has significant adverse impacts on marine ecosystems.However,identifying the main constituents of chemical mixtures that pose ecological threats is challenging due to the necessity of an integrated workflow for comprehensive identification and toxicological prioritization of pollutants.Here,an all-in-one mass spectrometric strategy integrating target,suspect,and nontarget analysis was used to investigate organic pollutants of concern in fishing port sediments,with 355 pollutants(32 from target analysis,118 from suspect screening and 205 from nontarget analysis)identified in 11 categories.The chemical classes of polycyclic aromatic hydrocarbons(PAHs),pesticides,and intermediates were the extensively detected chemical classes.The ecological risks of absolutely quantified pollutants(i.e.,16 parent PAHs,7 organophosphate esters(OPEs),10 pesticides and 4 benzotriazole ultraviolet absorbers)were assessed using toxicity-weighted concentration ranking,with o,p’-DDT being the major contributor.Under the toxicological priority index(ToxPi)framework,an extended ranking of all identified pollutants was achieved by combining instrument response and detection frequency,with a priority control list of 15 pollutants obtained,of which benzo[ghi]perylene(BghiP)and p,p’-DDE had the highest risk priority.Due to frequent detection rates and significant environmental risks,routine monitoring of petroleum pollutants is considered essential.This study presents a general workflow that includes comprehensive identification and prioritization of pollutants,facilitating chemical management and ecological risk assessment.展开更多
The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the inter...The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and porosity.Herein,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions.Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks.Furthermore,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/g.As proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66.This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.展开更多
Polycyclic aromatic hydrocarbons (PAHs) investigation in different matrices has been reported largely,whereas reports on snow samples were limited.Snow,as the main matrix in the polar region,has an important study m...Polycyclic aromatic hydrocarbons (PAHs) investigation in different matrices has been reported largely,whereas reports on snow samples were limited.Snow,as the main matrix in the polar region,has an important study meaning.PAHs in snow samples were analyzed to investigate the distribution and contamination status of them in the Antarctic,as well as to provide some references for global migration of PAHs.Snow samples collected in Fildes Peninsula were enriched and separated by solid-phase membrane disks and eluted by methylene dichloride,then quantified by gas chromatography/mass spectrometry.All types of PAHs were detected except for Benzo(a)pyrene.Principal component analysis method was applied to characterize them.Three factors (Naphthalene,Fluorene and Phenanthrene) accounted for 60.57%,21.61% and 9.80%,respectively.The results showed that the major PAHs sources maybe the atmospheric transportation,and the combustion of fuel in Fildes Peninsula.The comparison of concentration and types of PAHs between accumulated snow and fresh snow showed that the main compound concentrations in accumulated snow samples were higher than those in fresh ones.The risk assessment indicated that the amount of PAHs in the snow samples would not lead to ecological risk.展开更多
In recent years, Dechloranes have been widely detected in the environment around the world.However, understanding and knowledge of Dechloranes in remote regions, such as the Arctic,remain lacking. Therefore, the conce...In recent years, Dechloranes have been widely detected in the environment around the world.However, understanding and knowledge of Dechloranes in remote regions, such as the Arctic,remain lacking. Therefore, the concentrations of 5 Dechloranes in surface seawater, sediment,soil, moss, and dung collected from Ny-lesund in the Arctic were measured with the concentrations 93 pg/L, 342, 325, 1.4, and 258 pg/g, respectively, which were much lower than those in Asian and European regions. The mean ratios of anti-Dechlorane Plus(DP) to total DP(fanti) in seawater, sediment, soil, moss, dung, and atmospheric samples were 0.36, 0.21, 0.18,0.27, 0.66, and 0.43, respectively. Results suggested that the main source of DP in seawater,sediment, soil, and moss was long-range atmospheric transport. However, the ratio identified in dung was different, for which the migration behavior of the organism is probably the main source of DP.展开更多
Concentrations of 16 polybrominated diphenyl ether(PBDE) congeners were measured in river sediments, paddy soils and three species of paddy-field organisms(crab, loach and carp) collected from the Liaohe River Bas...Concentrations of 16 polybrominated diphenyl ether(PBDE) congeners were measured in river sediments, paddy soils and three species of paddy-field organisms(crab, loach and carp) collected from the Liaohe River Basin, northeastern China. The total contents of PBDEs(∑_(16)PBDEs) in sediments and paddy soils were in the ranges of 273.4–3246.3 pg/g dry weight(dw), and 192.1–1783.8 pg/g dw, respectively. BDE 209 was the dominant congener both in sediments and paddy soils. The concentrations of ∑_(16)PBDEs in sediments were significantly higher than those in the adjacent paddy soils, indicating a potential transport of PBDEs from river to paddy ecosystems via river water irrigation. The biota–soil accumulation factor(BSAF) was calculated as the ratio between the lipid-normalized concentration in paddyfield organisms and the total organic carbon-normalized concentration in paddy soil. The average BSAF values of ∑15PBDEs followed the sequence of crab(3.6) 〉 loach(3.3) 〉 carp(2.1). BDE 154 had the highest BSAF value, and a parabolic trend between BSAF values of individual PBDE congeners and their log KOWvalues was observed. In view of the fact that crab had the larger BSAF value and higher lipid content, the ecological risk and health risk for crab cultivation in paddy fields should be of particular concern.展开更多
Lidar techniques present a distinctive ability to resolve vertical structure of optical properties within the upper water column at both day-and night-time.However,accuracy challenges remain for existing lidar instrum...Lidar techniques present a distinctive ability to resolve vertical structure of optical properties within the upper water column at both day-and night-time.However,accuracy challenges remain for existing lidar instruments due to the ill-posed nature of elastic backscatter lidar retrievals and multiple scattering.Here we demonstrate the high performance of,to the best of our knowledge,the first shipborne oceanic high-spectral-resolution lidar(HSRL)and illustrate a multiple scattering correction algorithm to rigorously address the above challenges in estimating the depth-resolved diffuse attenuation coefficient Kd and the particulate backscattering coefficient bbp at 532 nm.HSRL data were collected during day-and night-time within the coastal areas of East China Sea and South China Sea,which are connected by the Taiwan Strait.Results include vertical profiles from open ocean waters to moderate turbid waters and first lidar continuous observation of diel vertical distribution of thin layers at a fixed station.The root-mean-square relative differences between the HSRL and coincident in situ measurements are 5.6%and 9.1%for Kd and bbp,respectively,corresponding to an improvement of 2.7-13.5 and 4.9-44.1 times,respectively,with respect to elastic backscatter lidar methods.Shipborne oceanic HSRLs with high performance are expected to be of paramount importance for the construction of 3D map of ocean ecosystem.展开更多
文摘The concentration and composition of nutrients,such as N,P,and Si,respond to biogeochemical processes and in turn,impact the phytoplanktons'community structure and primary production.In this study,historical data was systematically analyzed to identify long-term variations in nutrient trends,red tide frequency,phytoplankton community abundance,and dominant species succession in the southern Yellow Sea(SYS).Results showed that N/P concentration ratios dramatically increased as a function of increasing dissolved inorganic nitrogen concentrations,and Si/N concentration ratios were generally larger than 1,indicating that N limitation morphed to P limitation and potentially to Si limitation,which impacted the phytoplankton community.Furthermore,inter-annual trends over the past 50 years show that phytoplankton community abundance has been higher in spring and summer,relative to autumn and winter.Moreover,with respect to red tide frequency,diatom abundance gradually decreased,while that of dinoflagellates gradually increased.Dominant species succession showed that the phytoplankton community exhibited an evident tendency to transform from diatoms to dinoflagellates.These research results clearly depict the presence of an important correlation between the phytoplankton community and nutrient structure in the SYS.
基金The National Key Research and Development Program of China under contract No.2016YFC1402305the Postdoctoral Research Foundation of China under contract No.2016M601148the Scientific Research Special Fund of Marine Public Welfare Industry under contract No.201305002
文摘Parent and alkylated polycyclic aromatic hydrocarbons(alkyl-PAHs),which are a class of important toxic components of crude oil especially in the marine environment,exhibit adverse effects on aquatic life and potentially pose a human health risk.However,the lack of chronic toxicity data is one of the hindrances for alkylPAHs when assessing their ecological risks.In this study,predicted no-effect concentrations(PNECs)in seawater and marine sediment for ten parent-and alkyl-PAHs were derived by applying species sensitivity distributions(SSDs)and quantitative structure-activity relationships(QSARs).The local area,Dalian Bay,where an oil-spilled accident happened in 2010,was chosen as a case site to assess ecological risks for ten PAHs in surface seawaters and marine sediments.Their PNECs in seawater and sediment for protecting aquatic organisms in marine ecosystems were calculated and recommended in the range of 0.012-2.79μg/L and 48.2-1337 ng/g(dry weight),respectively.Overall,the derived PNECs for the studied PAHs in seawater and marine sediment were comparable to those obtained by classical methods.Risk quotient results indicate low ecological risks to ecosystems for ten parent-and alkyl-PAHs in surface seawaters and surface sediments from the Dalian Bay.These findings provide a first insight into the PNECs and ecological risks of alkyl-PAHs,emphasizing the role of the computational toxicology in ecological risk assessments.The use of QSARs has been identified as a valuable tool for preliminarily assessing ecological risks of emerging pollutants,being more predictable of real exposure scenarios for risk assessment purposes.
基金supported by the National Key Research and Development Program(2022YFC3105500)the National Natural Science Foundation of China(42206159)the Dalian Young Star of Science and Technology Project(2022RQ052).
文摘Environmental pollution from synthetic chemical mixtures has significant adverse impacts on marine ecosystems.However,identifying the main constituents of chemical mixtures that pose ecological threats is challenging due to the necessity of an integrated workflow for comprehensive identification and toxicological prioritization of pollutants.Here,an all-in-one mass spectrometric strategy integrating target,suspect,and nontarget analysis was used to investigate organic pollutants of concern in fishing port sediments,with 355 pollutants(32 from target analysis,118 from suspect screening and 205 from nontarget analysis)identified in 11 categories.The chemical classes of polycyclic aromatic hydrocarbons(PAHs),pesticides,and intermediates were the extensively detected chemical classes.The ecological risks of absolutely quantified pollutants(i.e.,16 parent PAHs,7 organophosphate esters(OPEs),10 pesticides and 4 benzotriazole ultraviolet absorbers)were assessed using toxicity-weighted concentration ranking,with o,p’-DDT being the major contributor.Under the toxicological priority index(ToxPi)framework,an extended ranking of all identified pollutants was achieved by combining instrument response and detection frequency,with a priority control list of 15 pollutants obtained,of which benzo[ghi]perylene(BghiP)and p,p’-DDE had the highest risk priority.Due to frequent detection rates and significant environmental risks,routine monitoring of petroleum pollutants is considered essential.This study presents a general workflow that includes comprehensive identification and prioritization of pollutants,facilitating chemical management and ecological risk assessment.
基金the National Natural Science Foundation of China(52125002)the Research Program of Chongqing Municipal Education Commission(KJZD-K202101502)the Natural Science Foundation of Jiangxi Province(20224ACB203015)。
基金the National Natural Science Foundation of China(Nos.52125002 and 51908270)the Natural Science Foundation of Jiangxi Province(No.20212ACB213006),and the National Key Research and Development Program of China(No.2019YFC1907900).
文摘The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and porosity.Herein,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions.Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks.Furthermore,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/g.As proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66.This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.
基金supported by the State Ocean Administration Young Scientists Research Program of China (No.2009507)the China Marine Public-welfare Program (No.200805095,201105013)
文摘Polycyclic aromatic hydrocarbons (PAHs) investigation in different matrices has been reported largely,whereas reports on snow samples were limited.Snow,as the main matrix in the polar region,has an important study meaning.PAHs in snow samples were analyzed to investigate the distribution and contamination status of them in the Antarctic,as well as to provide some references for global migration of PAHs.Snow samples collected in Fildes Peninsula were enriched and separated by solid-phase membrane disks and eluted by methylene dichloride,then quantified by gas chromatography/mass spectrometry.All types of PAHs were detected except for Benzo(a)pyrene.Principal component analysis method was applied to characterize them.Three factors (Naphthalene,Fluorene and Phenanthrene) accounted for 60.57%,21.61% and 9.80%,respectively.The results showed that the major PAHs sources maybe the atmospheric transportation,and the combustion of fuel in Fildes Peninsula.The comparison of concentration and types of PAHs between accumulated snow and fresh snow showed that the main compound concentrations in accumulated snow samples were higher than those in fresh ones.The risk assessment indicated that the amount of PAHs in the snow samples would not lead to ecological risk.
基金supported by the National Natural Science Foundation of China (No. 21377032)the Chinese Polar Environment Comprehensive Investigation and Assessment Program (Nos. 2014-02-01, 2014-03-04, 2014-04-01, 2014-04-03)+1 种基金the Marine Public Welfare Scientific Research Projects (No. 201105013)the Foundation of Polar Science Key Laboratory, SOA, China (No. KP201208)
文摘In recent years, Dechloranes have been widely detected in the environment around the world.However, understanding and knowledge of Dechloranes in remote regions, such as the Arctic,remain lacking. Therefore, the concentrations of 5 Dechloranes in surface seawater, sediment,soil, moss, and dung collected from Ny-lesund in the Arctic were measured with the concentrations 93 pg/L, 342, 325, 1.4, and 258 pg/g, respectively, which were much lower than those in Asian and European regions. The mean ratios of anti-Dechlorane Plus(DP) to total DP(fanti) in seawater, sediment, soil, moss, dung, and atmospheric samples were 0.36, 0.21, 0.18,0.27, 0.66, and 0.43, respectively. Results suggested that the main source of DP in seawater,sediment, soil, and moss was long-range atmospheric transport. However, the ratio identified in dung was different, for which the migration behavior of the organism is probably the main source of DP.
基金supported by the Chinese Public Welfare Projects on Environmental Protection (No. 201309030)the National Natural Science Foundation of China (Nos. 21077102 and 41201491)
文摘Concentrations of 16 polybrominated diphenyl ether(PBDE) congeners were measured in river sediments, paddy soils and three species of paddy-field organisms(crab, loach and carp) collected from the Liaohe River Basin, northeastern China. The total contents of PBDEs(∑_(16)PBDEs) in sediments and paddy soils were in the ranges of 273.4–3246.3 pg/g dry weight(dw), and 192.1–1783.8 pg/g dw, respectively. BDE 209 was the dominant congener both in sediments and paddy soils. The concentrations of ∑_(16)PBDEs in sediments were significantly higher than those in the adjacent paddy soils, indicating a potential transport of PBDEs from river to paddy ecosystems via river water irrigation. The biota–soil accumulation factor(BSAF) was calculated as the ratio between the lipid-normalized concentration in paddyfield organisms and the total organic carbon-normalized concentration in paddy soil. The average BSAF values of ∑15PBDEs followed the sequence of crab(3.6) 〉 loach(3.3) 〉 carp(2.1). BDE 154 had the highest BSAF value, and a parabolic trend between BSAF values of individual PBDE congeners and their log KOWvalues was observed. In view of the fact that crab had the larger BSAF value and higher lipid content, the ecological risk and health risk for crab cultivation in paddy fields should be of particular concern.
基金This study was supported by Excellent Young Scientist Program of Zhejang Provincial Natural Science Foundation of China(LR19D050001)National Key ResearchandDevelopment Programof China(2016YFC1400900)+1 种基金Fundamental Research Funds for the Central Universities(international team)Scientific Research Foundation for Talent Introduction(20201203Z0175,20201203Z0177)of Zhejiang University Ningbo Campus.
文摘Lidar techniques present a distinctive ability to resolve vertical structure of optical properties within the upper water column at both day-and night-time.However,accuracy challenges remain for existing lidar instruments due to the ill-posed nature of elastic backscatter lidar retrievals and multiple scattering.Here we demonstrate the high performance of,to the best of our knowledge,the first shipborne oceanic high-spectral-resolution lidar(HSRL)and illustrate a multiple scattering correction algorithm to rigorously address the above challenges in estimating the depth-resolved diffuse attenuation coefficient Kd and the particulate backscattering coefficient bbp at 532 nm.HSRL data were collected during day-and night-time within the coastal areas of East China Sea and South China Sea,which are connected by the Taiwan Strait.Results include vertical profiles from open ocean waters to moderate turbid waters and first lidar continuous observation of diel vertical distribution of thin layers at a fixed station.The root-mean-square relative differences between the HSRL and coincident in situ measurements are 5.6%and 9.1%for Kd and bbp,respectively,corresponding to an improvement of 2.7-13.5 and 4.9-44.1 times,respectively,with respect to elastic backscatter lidar methods.Shipborne oceanic HSRLs with high performance are expected to be of paramount importance for the construction of 3D map of ocean ecosystem.