Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging and nonpersistent contaminants.In this study,27 PPCPs in various water samples were extracted by solid phase extraction(SPE),and determin...Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging and nonpersistent contaminants.In this study,27 PPCPs in various water samples were extracted by solid phase extraction(SPE),and determined by isotope dilution method using liquid chromatography coupled to tandem triple quadruple mass spectrometer(LC-MS/MS).A total of 27 isotopically labeled standards(ILSs)were applied to correct the concentration of PPCPs in spiked ultrapure water,drinking water,river,effluent and influent sewage.The corrected recoveries were 73%-122%with the relative standard deviation(RSD)<16%,except for acetaminophen.The matrix effect for all kinds of water samples was<22%and the method quantitation limits(MQLs)were 0.45-8.6 ng/L.The developed method was successfully applied on environmental water samples.The SPE extracts of spiked ultrapure water,drinking water,river and wastewater effluent were stored for 70 days,and the ILSscorrected recoveries of 27 PPCPs were obtained to evaluate the correction ability of ILSs in the presence of variety interferences.The recoveries of 27 PPCPs over 70 days were within the scope of 72%-140%with the recovery variation<37%in all cases.The isotope dilution method seems to be of benefit when the extract has to be stored for long time before the instrument analysis.展开更多
Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging environmental contaminants,due to their inherent ability to induce physiological effects in human at low doses.An increasing number of st...Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging environmental contaminants,due to their inherent ability to induce physiological effects in human at low doses.An increasing number of studies has confirmed the presence of various PPCPs in different environmental compartments,which raises concerns about the potential adverse effects to humans and wildlife.Therefore,this article reviews the current state-of-knowledge on PPCPs in the freshwater aquatic environment.The environmental risk posed by these contaminants is evaluated in light of the persistence,bioaccumulation and toxicity criteria.Available literature on the sources,transport and degradation of PPCPs in the aquatic environment are evaluated,followed by a comprehensive review of the reported concentrations of different PPCP groups in the freshwater aquatic environment(water,sediment and biota)of the five continents.Finally,future perspectives for research on PPCPs in the freshwater aquatic environment are discussed in light of the identified research gaps in current knowledge.展开更多
药物和个人护理用品(pharmaceutical and personal care products, PPCPs)作为一类新兴的污染物,在环境中的存在、迁移已引起特别关注,成为环境领域热点研究方向。综述液相色谱-质谱联用、气相色谱-质谱联用两类分析检测技术的选择、应...药物和个人护理用品(pharmaceutical and personal care products, PPCPs)作为一类新兴的污染物,在环境中的存在、迁移已引起特别关注,成为环境领域热点研究方向。综述液相色谱-质谱联用、气相色谱-质谱联用两类分析检测技术的选择、应用和发展,风险评价重难点和风险评价方法的选择,活性污泥法、膜处理工艺、碳吸附法等常用控制技术的研究进展。指出水环境中PPCPs污染物识别的标准体系不完善、方法不统一,风险评价无法全面、客观与准确地反映PPCPs的生态影响,控制技术还需进一步加强和提升。展开更多
There is continued interest in the occurrence and monitoring of emerging contaminants(ECs)in wastewater treatment plants(WWTPs)to assess their potential impact when released into the environment.The objective of this ...There is continued interest in the occurrence and monitoring of emerging contaminants(ECs)in wastewater treatment plants(WWTPs)to assess their potential impact when released into the environment.The objective of this study was to determine the occurrence of pharmaceutical and personal care products(PPCPs)in WWTP influents and effluents and receiving river waters in Pretoria,South Africa.Targeted screening and identification of PPCPs in the samples was done using liquid chromatography(LC)coupled with high resolution mass spectrometry(HRMS)Orbitrap™HRMS,after clean-up and preconcentration with Waters Oasis®hydrophilic-lipophilic-balanced(HLB)solid phase extraction(SPE)cartridges.Of the 156 target analytes screened in the study,120 could be satisfactorily determined under the study conditions,with 71 and 73 compounds being detected and quantified in the influent and effluent samples,respectively.Concentrations in the influents ranged from<ILOQ-14.2 mgL^-1and those in the effluent from<ILOQ-2.45 mgL^-1.It was found that 84%of the quantified compounds belonged to various classes of pharmaceuticals.Ibuprofen,caffeine,paracetamol and estradiol were the major individual contaminants in influent samples with average concentrations of 14.2,8.68,4.79 and 1.02 mgL^-1,respectively.In the effluent samples,the highest concentrations were recorded for estradiol(2.45 mgL^-1),ibuprofen(1.03 mgL^-1)and efavirenz(0.58 mgL^-1).The highest mean concentrations(above 0.5 mgL^-1)recorded in the river water samples were for ibuprofen,(4.14 mgL^-1downstream;3.19 mgL^-1upstream),caffeine(2.98 mgL^-1downstream;1.42 mgL^-1upstream),paraxanthine(1.22 mgL^-1downstream;0.798 mgL^-1upstream).Analysis of river water samples also revealed that PPCP contamination in the river system cannot be solely attributed to the WWTP effluents.Twenty-four compounds presented in this study are reported for the first time in South African surface waters.展开更多
药物与个人护理品(pharmaceuticals and personal care products,PPCPs)的污染和环境归趋问题备受关注。其中厌氧降解转化作为疏水性PPCPs在自然环境介质中的主要消解方式尤为重要。本文以典型PPCPs为例,分析了城市污水处理厌氧工艺对PP...药物与个人护理品(pharmaceuticals and personal care products,PPCPs)的污染和环境归趋问题备受关注。其中厌氧降解转化作为疏水性PPCPs在自然环境介质中的主要消解方式尤为重要。本文以典型PPCPs为例,分析了城市污水处理厌氧工艺对PPCPs的去除情况,主要包括污泥吸附和厌氧生物转化;总结了化学结构、微生物、碳源和氧化还原电位等多种因素对PPCPs厌氧降解转化效率的影响,其中氧化还原电位发挥重要作用,因其与氧化还原酶密切相关;同时,重点归纳了磺胺甲噁唑、苯并三唑和三氯生等3种典型PPCPs在不同氧化还原电位下的厌氧降解转化途径,并对PPCPs厌氧微生物降解的未来研究重点和发展方向进行展望:(1)强化PPCPs的有机质-厌氧微生物共代谢降解机制研究;(2)聚焦PPCPs厌氧降解菌群筛选及其功能研究;(3)深入开展厌氧降解菌群培养体系构建和原位厌氧降解研究。本研究相关结果有望为PPCPs的污染防治提供科学依据。展开更多
Pharmaceutical and personal care products(PPCPs)and corresponding transformation products have caused widespread concern due to their persistent emissions and potential toxicity.They have wide octanol-water partition ...Pharmaceutical and personal care products(PPCPs)and corresponding transformation products have caused widespread concern due to their persistent emissions and potential toxicity.They have wide octanol-water partition coefficients(K_(ow))and different ionization constants(pK_(a))resulting in a poor analysis accuracy and efficiency.A suitable analytical method is the first prerequisite for further research on their environmental behavior to prioritize the substances.This study reviewed a full-scale analytical protocol for environmental samples in the recent ten years:from sampling to instrumental methods.Passive sampling techniques were compared and recommended for long-term continuous and scientific observation.A quick and effective sample extraction and clean-up method are highly required.Chromatographic methods coupled to mass spectrometry for determining PPCPs with a wide range of logK_(ow)(-7.53 to 10.80)were summed up.High-resolution mass spectrometry was confirmed to be a promising strategy for screening unknown transformation products,which would provide a nanogram level of detection limits and more accurate mass resolution.Screening strategies and mass change principles were summarized in detail.The recovery rate was important in multiple contaminants analysis identification and factors affecting the recovery rate of PPCPs were also discussed in this review,including sample matrix,target compounds characteristics,extraction method and solid-phase adsorbent.This review provides useful information for the selection of appropriate analytical methods and future development directions.展开更多
A simple, facile in situ reduction approach is reported for the synthesis of Pd- nanoparticle-decorated phosphotungstic acid （PTA）-MIL-100（Fe） nanocomposites （Pd-H3PW12040-MIL-100（Fe）, denoted Pd-PTA-MIL-100（F...A simple, facile in situ reduction approach is reported for the synthesis of Pd- nanoparticle-decorated phosphotungstic acid （PTA）-MIL-100（Fe） nanocomposites （Pd-H3PW12040-MIL-100（Fe）, denoted Pd-PTA-MIL-100（Fe））. During the in situ synthesis, PTA is encapsulated into the matrix of MIL-100（Fe） and serves as a UV-switchable reducing agent, resulting in highly dispersed Pd NPs. Using the photocatalytic degradation of pharmaceuticals and personal care products as model reactions, the ternary Pd-PTA-MIL-100（Fe） hybrids exhibited enhanced photocatalytic activity compared with their foundation matrices, the binary PTA-MIL-100（Fe） nanocomposite. Based on photoelectrochemical analyses, the improved photocatalytic performance can be attributed to the well-known electronic conductivity of the Pd NPs, the fast electron transport of PTA, the intense visible-light absorption of MIL-100（Fe）, and the matched energy levels of the three components： MIL-100（Fe）, PTA, and Pd NPs. Importantly, almost no Fe and W ions were leached from the samples during the reaction, demonstrating the photostability of the Pd-PTA-MIL-100（Fe） composite. In addition, possible photocatalytic reactions mechanisms have also been investigated.展开更多
In this study,a hydrophilic resin named GCHM was fabricated based on poly(N-vinyl pyrrolidone-codivinylbenzene),characterized,and applied as a solid-phase extraction(SPE)material.Up to 44 pharmaceuticals and personal ...In this study,a hydrophilic resin named GCHM was fabricated based on poly(N-vinyl pyrrolidone-codivinylbenzene),characterized,and applied as a solid-phase extraction(SPE)material.Up to 44 pharmaceuticals and personal care products(PPCPs)belonging to 10 classes were recovered in environmental water samples.Different variables affecting extraction,such as adsorbent amount,sample pH,and loading speed,were optimized.Under optimal conditions,the average absolute recovgy of 44 PPCPs was 75.6%using GCHM,indicating a better performance than the commercial Oasis^HLB.SPE with home-made hydrophilic polymeric sorbent followed by ultra-performance liquid chromatography and tandem mass spectrometry was validated,and the method achieved good linearity(r2>0.991,for all analytes).In addition,the method detection limits of target compounds ranged from 0.03 to 0.6 ng/L.The developed method was applied to determine PPCPs in 10 environmental water samples taken from the Yangtze River,Huaihe River,and Taihu Lake,1 groundwater sample from Changzhou in Jiangsu Province,1 wastewater sample from Xiamen and 2 seawater samples from the Jiulong River in Fujian Province,China.In these samples,22 compounds were determined at levels ranging from 0.5 to 1590 ng/L.展开更多
The presence of pharmaceuticals and personal care products(PPCPs)in the aquatic environment may pose potential threat to the ecosystem and human health,hence PPCPs have aroused much concern over the world.The contamin...The presence of pharmaceuticals and personal care products(PPCPs)in the aquatic environment may pose potential threat to the ecosystem and human health,hence PPCPs have aroused much concern over the world.The contamination of PPCPs in the groundwater,the main source of drinking water supply in many countries and regions,has been extensively studied in the last decade.This paper reviews the occurrence of frequently detected PPCPs,including antibiotics,anti-inflammatories,lipid-regulators,carbamazepine,caffeine,and N,N-diethyl-m-toluamide in groundwater,with special concern to the progress made over the past three years.Possible emission sources for PPCPs in groundwater,such as wastewater and contaminated surface water,landfills,septic systems,livestock breeding and sewer leakage,are summarized.Besides,adsorption,migration and degradation,the dominant mechanisms in the subsurface transport and fate of PPCPs,are discussed,and the insights into the future study of PPCPs in the groundwater are provided.展开更多
基金This work was supported by the Major Science and Technology Program for Water Pollution Control and Treatment in China(Nos.2017ZX07202-001 and 2017ZX07202-004).
文摘Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging and nonpersistent contaminants.In this study,27 PPCPs in various water samples were extracted by solid phase extraction(SPE),and determined by isotope dilution method using liquid chromatography coupled to tandem triple quadruple mass spectrometer(LC-MS/MS).A total of 27 isotopically labeled standards(ILSs)were applied to correct the concentration of PPCPs in spiked ultrapure water,drinking water,river,effluent and influent sewage.The corrected recoveries were 73%-122%with the relative standard deviation(RSD)<16%,except for acetaminophen.The matrix effect for all kinds of water samples was<22%and the method quantitation limits(MQLs)were 0.45-8.6 ng/L.The developed method was successfully applied on environmental water samples.The SPE extracts of spiked ultrapure water,drinking water,river and wastewater effluent were stored for 70 days,and the ILSscorrected recoveries of 27 PPCPs were obtained to evaluate the correction ability of ILSs in the presence of variety interferences.The recoveries of 27 PPCPs over 70 days were within the scope of 72%-140%with the recovery variation<37%in all cases.The isotope dilution method seems to be of benefit when the extract has to be stored for long time before the instrument analysis.
文摘Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging environmental contaminants,due to their inherent ability to induce physiological effects in human at low doses.An increasing number of studies has confirmed the presence of various PPCPs in different environmental compartments,which raises concerns about the potential adverse effects to humans and wildlife.Therefore,this article reviews the current state-of-knowledge on PPCPs in the freshwater aquatic environment.The environmental risk posed by these contaminants is evaluated in light of the persistence,bioaccumulation and toxicity criteria.Available literature on the sources,transport and degradation of PPCPs in the aquatic environment are evaluated,followed by a comprehensive review of the reported concentrations of different PPCP groups in the freshwater aquatic environment(water,sediment and biota)of the five continents.Finally,future perspectives for research on PPCPs in the freshwater aquatic environment are discussed in light of the identified research gaps in current knowledge.
文摘药物和个人护理用品(pharmaceutical and personal care products, PPCPs)作为一类新兴的污染物,在环境中的存在、迁移已引起特别关注,成为环境领域热点研究方向。综述液相色谱-质谱联用、气相色谱-质谱联用两类分析检测技术的选择、应用和发展,风险评价重难点和风险评价方法的选择,活性污泥法、膜处理工艺、碳吸附法等常用控制技术的研究进展。指出水环境中PPCPs污染物识别的标准体系不完善、方法不统一,风险评价无法全面、客观与准确地反映PPCPs的生态影响,控制技术还需进一步加强和提升。
基金the Water Research Commission(WRC Project No.K5-2516)for financial support for the project.
文摘There is continued interest in the occurrence and monitoring of emerging contaminants(ECs)in wastewater treatment plants(WWTPs)to assess their potential impact when released into the environment.The objective of this study was to determine the occurrence of pharmaceutical and personal care products(PPCPs)in WWTP influents and effluents and receiving river waters in Pretoria,South Africa.Targeted screening and identification of PPCPs in the samples was done using liquid chromatography(LC)coupled with high resolution mass spectrometry(HRMS)Orbitrap™HRMS,after clean-up and preconcentration with Waters Oasis®hydrophilic-lipophilic-balanced(HLB)solid phase extraction(SPE)cartridges.Of the 156 target analytes screened in the study,120 could be satisfactorily determined under the study conditions,with 71 and 73 compounds being detected and quantified in the influent and effluent samples,respectively.Concentrations in the influents ranged from<ILOQ-14.2 mgL^-1and those in the effluent from<ILOQ-2.45 mgL^-1.It was found that 84%of the quantified compounds belonged to various classes of pharmaceuticals.Ibuprofen,caffeine,paracetamol and estradiol were the major individual contaminants in influent samples with average concentrations of 14.2,8.68,4.79 and 1.02 mgL^-1,respectively.In the effluent samples,the highest concentrations were recorded for estradiol(2.45 mgL^-1),ibuprofen(1.03 mgL^-1)and efavirenz(0.58 mgL^-1).The highest mean concentrations(above 0.5 mgL^-1)recorded in the river water samples were for ibuprofen,(4.14 mgL^-1downstream;3.19 mgL^-1upstream),caffeine(2.98 mgL^-1downstream;1.42 mgL^-1upstream),paraxanthine(1.22 mgL^-1downstream;0.798 mgL^-1upstream).Analysis of river water samples also revealed that PPCP contamination in the river system cannot be solely attributed to the WWTP effluents.Twenty-four compounds presented in this study are reported for the first time in South African surface waters.
文摘药物与个人护理品(pharmaceuticals and personal care products,PPCPs)的污染和环境归趋问题备受关注。其中厌氧降解转化作为疏水性PPCPs在自然环境介质中的主要消解方式尤为重要。本文以典型PPCPs为例,分析了城市污水处理厌氧工艺对PPCPs的去除情况,主要包括污泥吸附和厌氧生物转化;总结了化学结构、微生物、碳源和氧化还原电位等多种因素对PPCPs厌氧降解转化效率的影响,其中氧化还原电位发挥重要作用,因其与氧化还原酶密切相关;同时,重点归纳了磺胺甲噁唑、苯并三唑和三氯生等3种典型PPCPs在不同氧化还原电位下的厌氧降解转化途径,并对PPCPs厌氧微生物降解的未来研究重点和发展方向进行展望:(1)强化PPCPs的有机质-厌氧微生物共代谢降解机制研究;(2)聚焦PPCPs厌氧降解菌群筛选及其功能研究;(3)深入开展厌氧降解菌群培养体系构建和原位厌氧降解研究。本研究相关结果有望为PPCPs的污染防治提供科学依据。
基金supported by the National Natural Science Foundation of China(No.41977142)the Major Science and Technology Program for Water Pollution Control and Treatment(No.2018ZX07111003)+1 种基金the Key Technologies Research and Development Program(No.2019YFC1806104)the Fundamental Research Funds for the Central Universities(No.JD2006)。
文摘Pharmaceutical and personal care products(PPCPs)and corresponding transformation products have caused widespread concern due to their persistent emissions and potential toxicity.They have wide octanol-water partition coefficients(K_(ow))and different ionization constants(pK_(a))resulting in a poor analysis accuracy and efficiency.A suitable analytical method is the first prerequisite for further research on their environmental behavior to prioritize the substances.This study reviewed a full-scale analytical protocol for environmental samples in the recent ten years:from sampling to instrumental methods.Passive sampling techniques were compared and recommended for long-term continuous and scientific observation.A quick and effective sample extraction and clean-up method are highly required.Chromatographic methods coupled to mass spectrometry for determining PPCPs with a wide range of logK_(ow)(-7.53 to 10.80)were summed up.High-resolution mass spectrometry was confirmed to be a promising strategy for screening unknown transformation products,which would provide a nanogram level of detection limits and more accurate mass resolution.Screening strategies and mass change principles were summarized in detail.The recovery rate was important in multiple contaminants analysis identification and factors affecting the recovery rate of PPCPs were also discussed in this review,including sample matrix,target compounds characteristics,extraction method and solid-phase adsorbent.This review provides useful information for the selection of appropriate analytical methods and future development directions.
文摘A simple, facile in situ reduction approach is reported for the synthesis of Pd- nanoparticle-decorated phosphotungstic acid （PTA）-MIL-100（Fe） nanocomposites （Pd-H3PW12040-MIL-100（Fe）, denoted Pd-PTA-MIL-100（Fe））. During the in situ synthesis, PTA is encapsulated into the matrix of MIL-100（Fe） and serves as a UV-switchable reducing agent, resulting in highly dispersed Pd NPs. Using the photocatalytic degradation of pharmaceuticals and personal care products as model reactions, the ternary Pd-PTA-MIL-100（Fe） hybrids exhibited enhanced photocatalytic activity compared with their foundation matrices, the binary PTA-MIL-100（Fe） nanocomposite. Based on photoelectrochemical analyses, the improved photocatalytic performance can be attributed to the well-known electronic conductivity of the Pd NPs, the fast electron transport of PTA, the intense visible-light absorption of MIL-100（Fe）, and the matched energy levels of the three components： MIL-100（Fe）, PTA, and Pd NPs. Importantly, almost no Fe and W ions were leached from the samples during the reaction, demonstrating the photostability of the Pd-PTA-MIL-100（Fe） composite. In addition, possible photocatalytic reactions mechanisms have also been investigated.
基金Authors gratefully acknowledge the generous support provided by the National Key R&D Program of China(Grant No.2016YFE0112300)the National Natural Science Foundation of China(Grant Nos.51678290,51438008 and 51778281)+3 种基金Jiangsu Natural Science Fund,China(No.B K 20171342)Jiangsu Provincial Key Medical Discipline(Laboratory)of China(No.Z D X K A 2016008)Jiangsu Preventive Medicine Project of China(No.Y2018081)The authors also thank Dr.Zhe Wang from Nanyang Technological University(Singapore)for his support on this project.
文摘In this study,a hydrophilic resin named GCHM was fabricated based on poly(N-vinyl pyrrolidone-codivinylbenzene),characterized,and applied as a solid-phase extraction(SPE)material.Up to 44 pharmaceuticals and personal care products(PPCPs)belonging to 10 classes were recovered in environmental water samples.Different variables affecting extraction,such as adsorbent amount,sample pH,and loading speed,were optimized.Under optimal conditions,the average absolute recovgy of 44 PPCPs was 75.6%using GCHM,indicating a better performance than the commercial Oasis^HLB.SPE with home-made hydrophilic polymeric sorbent followed by ultra-performance liquid chromatography and tandem mass spectrometry was validated,and the method achieved good linearity(r2>0.991,for all analytes).In addition,the method detection limits of target compounds ranged from 0.03 to 0.6 ng/L.The developed method was applied to determine PPCPs in 10 environmental water samples taken from the Yangtze River,Huaihe River,and Taihu Lake,1 groundwater sample from Changzhou in Jiangsu Province,1 wastewater sample from Xiamen and 2 seawater samples from the Jiulong River in Fujian Province,China.In these samples,22 compounds were determined at levels ranging from 0.5 to 1590 ng/L.
基金supported by the National Natural Science Foundation(51208199,51408425)the Fundamental Research Funds for the Central Universities(22A201514057)+1 种基金Beijing Key Laboratory for Emerging Organic Contaminants Control,the Foundation of The State Key Laboratory of Pollution Control and Resource Reuse,China(PCRRG 11017)the Specialized Research Fund for the Doctoral Program of Higher Education of China(20130072120033).
文摘The presence of pharmaceuticals and personal care products(PPCPs)in the aquatic environment may pose potential threat to the ecosystem and human health,hence PPCPs have aroused much concern over the world.The contamination of PPCPs in the groundwater,the main source of drinking water supply in many countries and regions,has been extensively studied in the last decade.This paper reviews the occurrence of frequently detected PPCPs,including antibiotics,anti-inflammatories,lipid-regulators,carbamazepine,caffeine,and N,N-diethyl-m-toluamide in groundwater,with special concern to the progress made over the past three years.Possible emission sources for PPCPs in groundwater,such as wastewater and contaminated surface water,landfills,septic systems,livestock breeding and sewer leakage,are summarized.Besides,adsorption,migration and degradation,the dominant mechanisms in the subsurface transport and fate of PPCPs,are discussed,and the insights into the future study of PPCPs in the groundwater are provided.
