The membrane bioreactor(MBR)technology is a rising star for wastewater treatment.The pollutant elimination and membrane fouling performances of MBRs are essentially related to the dissolved organic matter(DOM)in the s...The membrane bioreactor(MBR)technology is a rising star for wastewater treatment.The pollutant elimination and membrane fouling performances of MBRs are essentially related to the dissolved organic matter(DOM)in the system.Three-dimensional excitation-emission matrix(3D-EEM)fluorescence spectroscopy,a powerful tool for the rapid and sensitive characterization of DOM,has been extensively applied in MBR studies;however,only a limited portion of the EEM fingerprinting information was utilized.This paper revisits the principles and methods of fluorescence EEM,and reviews the recent progress in applying EEM to characterize DOM in MBR studies.We systematically introduced the information extracted from EEM by considering the fluorescence peak location/intensity,wavelength regional distribution,and spectral deconvolution(giving fluorescent component loadings/scores),and discussed how to use the information to interpret the chemical compositions,physiochemical properties,biological activities,membrane retention/fouling behaviors,and migration/transformation fates of DOM in MBR systems.In addition to conventional EEM indicators,novel fluorescent parameters are summarized for potential use,including quantum yield,Stokes shift,excited energy state,and fluorescence lifetime.The current limitations of EEM-based DOM characterization are also discussed,with possible measures proposed to improve applications in MBR monitoring.展开更多
A novel approach is proposed for direct quantitative analysis of thiabendazole in the orange extract by using excitation-emission matrix fluorescence coupled with second-order calibration methods based on the alternat...A novel approach is proposed for direct quantitative analysis of thiabendazole in the orange extract by using excitation-emission matrix fluorescence coupled with second-order calibration methods based on the alternating trilinear decomposition(ATLD) and the alternating normalization-weighted error(ANWE) algorithms,respectively. The average recoveries of thiabendazole in the orange extract by using ATLD and ANWE with an estimated component number of two were 99.7 ± 3.3% and 103.5 ± 4.1%,respectively. Furthermore,the accuracy of the two algorithms was also evaluated through elliptical joint confidence region(EJCR) tests as well as figures of merit,such as sensitivity(SEN),selectivity(SEL) and limit of detection(LOD). The experimental results demonstrate that both algorithms have been satisfactorily applied to the determination of thiabendazole in orange extract,and the perform-ance of ANWE is slightly better than that of ATLD.展开更多
This study established back-propagation neural networks(BPNNs)for evaluating the freshness of bighead carp(Hypophthalmichthys nobilis)heads during chilled storage via fluorescence spectroscopy using an excitation-emis...This study established back-propagation neural networks(BPNNs)for evaluating the freshness of bighead carp(Hypophthalmichthys nobilis)heads during chilled storage via fluorescence spectroscopy using an excitation-emission matrix(EEM).The total volatile basic nitrogen(TVB-N)and total aerobic count(TAC)of fish increased obviously during storage at 0,4,8,12,and 16°C,while sensory scores decreased with increasing storage time.The EEM fluorescence intensity was measured,and its change was correlated with the freshness indicators of the samples.Three characteristic components of EEM data were extracted by parallel factor analysis,and two freshness indicators were used to construct the EEM-BPNNs model.The results demonstrated that the relative errors of the EEM-BPNNs model for TVB-N and TAC were less than 14%.This result indicated that the EEM-BPNNs model could determine the freshness of fish in cold chains in a rapid and nondestructive way.展开更多
The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to invest...The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to investigate the influence of transparent exopolymer particles(TEP)on the behavior of dissolved organic carbon(DOC)in this region,a comprehensive study was conducted,encompassing both open water areas and highly productive polynyas.It was found that microbial heterotrophic metabolism is the primary process responsible for the production of humic-like fluorescent components in the open ocean.The relationship between apparent oxygen utilization and the two humic-like components can be accurately described by a power-law function,with a conversion rate consistent with that observed globally.The presence of TEP was found to have little impact on this process.Additionally,the study revealed the accumulation of DOC at the sea surface in the Amundsen Sea Polynya,suggesting that TEP may play a critical role in this phenomenon.These findings contribute to a deeper understanding of the dynamics and surface accumulation of DOC in the Amundsen Sea Polynya,and provide valuable insights into the carbon cycle in this region.展开更多
To understand the aerosol characteristics in a regional background environment,fine-particle(PM_(2.5),n=228)samples were collected over a one-year period at the Shangdianzi(SDZ)station,which is a Global Atmospheric Wa...To understand the aerosol characteristics in a regional background environment,fine-particle(PM_(2.5),n=228)samples were collected over a one-year period at the Shangdianzi(SDZ)station,which is a Global Atmospheric Watch regional background station in North China.The chemical and optical characteristics of PM_(2.5)were analyzed,including organic carbon,elemental carbon,water-soluble organic carbon,water-soluble inorganic ions,and fluorescent components of watersoluble organic matter.The source factors of major aerosol components are apportioned,and the sources of the fluorescent chromophores are further analyzed.The major chemical components of PM_(2.5)at SDZ were NO_(3)^(-),organic matter,SO_(4)^(2-),and NH_(4)^(+).Annually,water-soluble organic carbon contributed 48%±15%to the total organic carbon.Secondary formation(52%)and fossil fuel combustion(63%)are the largest sources of water-soluble organic matter and water-insoluble organic matter,respectively.In addition,three humic-like and one protein-like matter were identified via parallel factor analysis for excitation–emission matrices.The fluorescence intensities of the components were highest in winter and lowest in summer,indicating the main impact of burning sources.This study contributes to understanding the chemical and optical characteristics of ambient aerosols in the background atmosphere.展开更多
Dissolved organic matter(DOM)plays a crucial role in both the carbon cycle and geochemical cycles of other nutrient elements,which is of importance to the management and protection of the aquatic environments.To achie...Dissolved organic matter(DOM)plays a crucial role in both the carbon cycle and geochemical cycles of other nutrient elements,which is of importance to the management and protection of the aquatic environments.To achieve a more comprehensive understanding the characteristics of DOM in the Changjiang(Yangtze)River basin,water samples from four natural lakes(Xiandao,Baoan,Daye,and Qingshan)in southeastern Hubei Province in China with different eutrophication levels were collected and analyzed.The optical characteristics were analyzed using ultraviolet-visible spectrophotometry and excitation-emission matrix spectroscopy coupled with parallel factor analysis.The results show that:(1)two humic-like components(C1 and C2)and two protein-like substances(C3 and C4)of DOM were identified in all waterbodies;(2)C3 originated primarily from the degradation of microalgae and contributed substantially to humic-like components during transformation.C4 was widely present in the Changjiang River basin and its formation was related to microbial activity,rather than algal blooms or seasons.Influenced by the water mixing,the protein-like components were more likely to be transformed by microorganism,whereas humic-like components were more easily to be photobleached;(3)the concentration of DOM and the fluorescence intensity of humic-like components gradually increased with rising lake eutrophication levels.With respect to protein-like components,only C3 showed changes along the eutrophication gradients;(4)DOM showed a high affinity with permanganate index(COD Mn)and chlorophyll a(chl a)while the relationship was variable with phosphorus.This study helps us systematically understand the DOM characteristics,microbial activities,and pollutant transformation in the Changjiang River basin and provides reference to the ecological restoration of aquatic environments.展开更多
Chromophoric dissolved organic matter(CDOM)is a key component of organic matter that contributes to the ecological functioning of lakes.The lakes in Taihu Lake Basin play an important role in maintaining regional ecol...Chromophoric dissolved organic matter(CDOM)is a key component of organic matter that contributes to the ecological functioning of lakes.The lakes in Taihu Lake Basin play an important role in maintaining regional ecological stabilities;however,the optical characteristics of the CDOM in the upstream and downstream lakes in this basin have not yet been systematically studied.Here,the optical characteristics of CDOM in ten lakes of upstream and downstream of the Taihu Lake Basin were studied using UV-Visible and excitation-emission matrix spectroscopies.Three different fluorophores consisting of two humic-like components(C1,C2)and one protein-like component(C3)were identified by parallel factor analysis.Soil or surface erosion was responsible for the higher abund-ance of C1 in the upstream lakes,and increased biological activities accounted for the higher abundance of C3 in the downstream lakes.Rainfall erosion in the wet season led to an increase in CDOM.We also found that the photodegradation and flocculation degree,which played a significant role in reducing CDOM,were higher in downstream lakes than in upstream lakes.Optical analysis of CDOM provides a promising method for monitoring water qualities(e.g.,total phosphorus and potassium permanganate index)in each lake.Re-ductions in soil or surface erosion in the upstream are needed to improve water quality.展开更多
Dissolved organic matter(DOM)in surface waters can vary markedly in character depending on seasonal variations such as rainfall intensity,UV radiations and temperature.Changes in DOM as well as temperature and rainfal...Dissolved organic matter(DOM)in surface waters can vary markedly in character depending on seasonal variations such as rainfall intensity,UV radiations and temperature.Changes in DOM as well as temperature and rainfall intensity over the year can affect the biochemical processes occurring in bank filtration(BF).Identification and characterization of DOM in the surface water could help to optimize the water treatment and provide stable and safe drinking water.This study investigated year-long variations of DOM concentrations and compositions in a surface water of a circulated outdoor pond(research facility)connected to a BF passage.DOM was dominated by humic substances and a changing pattern of DOM in surface water was observed throughout the year.A significant increase of DOM(~38%)in surface water was noted in August compared to November.The fluorescent DOM showed that DOM in summer was enriched with the degradable fraction whilst non-degradable fraction was dominated in winter.A constant(1.7±0.1 mg/L)effluent DOM was recirculated in the system throughout the year.DOM removal through BF varied between 4%to 39%and was achieved within a few meters after infiltration and significantly correlated with influent DOM concentration(R^(2)=0.82,p<0.05).However,no significant(p>0.05)change in the removal of DOM was observed in two subsurface layers(upper and lower).This study highlights the presence of a constant non-degradable DOM in the bank filtrate,which was not affected by temperature,redox conditions and UV radiations.展开更多
Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 veg...Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 vegetable fields in administrative regions of China' Mainland, of which 122 were selected for further investigation. DOM properties were characterized by three-dimensional excitation-emission matrix(3D-EEM) fuorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry(FTICRMS)(field intensity is 15 Tesla). Our results indicated that the main constituents were UVA humic-like substances, humic-like substances, fulvic acid-like substances, and tyrosine-like substances. A total of 10,989 molecular formulae with a mass range of 100.04 to 799.59 Da were detected, covering the mass spectrometric information of the soil samples from 27 different regions. CHO and CHON molecules were dominant in DOM, whereas lignin, tannins,and aromatic substances served as the main components. The results of cluster analysis revealed that the soil properties in Jiangxi Province were considerably different from those in other regions. The key backgrounds of the DOM molecular characteristics in the vegetablefield soil samples across China' Mainland were provided at the molecular level, with large abundance and great variability.展开更多
Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coex...Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coexist with Transition Metals(TMs)in PM,have been found to contribute to ROS formation.However,the interaction between WSOCs and TMs and its effect on ROS generation are still unknown.In this study,we examined the ROS concentrations of V,Zn,Suwannee River Fulvic Acid(SRFA),Suwannee River Humic Acid(SRHA)and the mixtures of V/Zn and SRFA/SRHA by using a cell-free 2’,7’-Dichlorodihydrofluorescein(DCFH)assay.The results showed that V or Zn synergistically promoted ROS generated by SRFA,but had an antagonistic effect on ROS generated by SRHA.Fluorescence quenching experiments indicated that V and Zn were more prone to form stable complexes with aromatic humic acid-like component(C1)and fulvic acidlike component(C3)in SRFA and SRHA.Results suggested that the underlying mechanism involving the fulvic acid-like component in SRFA more tending to complex with TMs to facilitate ROS generation throughπelectron transfer.Our work showed that the complexing ability and complexing stability of atmospheric PM organics with metals could significantly affect ROS generation.It is recommended that the research deploying multiple analytical methods to quantify the impact of PM components on public health and environment is needed in the future.展开更多
Molecular weight(Mw) is a fundamental property of humic acids(HAs), which considerably affect the mobility and speciation of heavy metals in the environment. In this study, soil humic acid(HA) extracted from Jinyun Mo...Molecular weight(Mw) is a fundamental property of humic acids(HAs), which considerably affect the mobility and speciation of heavy metals in the environment. In this study, soil humic acid(HA) extracted from Jinyun Mountain, Chongqing was ultra-filtered into four fractions according to the molecular weight, and their properties were characterized.Complexation of cadmium was investigated by titration experiments. For the first time,Langmuir and non-ideal competitive adsorption-Donna(NICA-Donnan) models combined with fluorescence excitation-emission matrix(EEM) quenching were employed to elucidate the binding characteristics of individual Mw fractions of HA. The results showed that the concentration of acidic functional groups decreased with increasing Mw, especially the phenolic groups. The humification degree and aliphaticity increased with increasing Mw as indicated by elemental composition analysis and FT-IR spectra. The binding capacity of Cd^(2+) to Mw fractions of HA followed the order UF1(< 5 kDa) > UF2(5–10 kDa) > UF4(> 30 kDa) > UF3(10–30 kDa). Moreover, the distribution of cadmium speciation indicated that the phenolic groups were responsible for the variations in binding of Cd^(2+) among different Mw fractions. The results of fluorescence quenching illustrated that the binding capacity of Cd^(2+) to Mw fractions was controlled by the content of functional groups, while the binding affinity was largely influenced by structural factors. The results provide a better understanding of the roles that different HA Mw fractions play in heavy metal binding,which has important implications in the control of heavy metal migration and bio-toxicity.展开更多
Although marine and terrestrial emissions simultaneously affect the formation of atmospheric fine particles in coastal areas,knowledge on the optical properties and sources of water-soluble matter in these areas is st...Although marine and terrestrial emissions simultaneously affect the formation of atmospheric fine particles in coastal areas,knowledge on the optical properties and sources of water-soluble matter in these areas is still scarce.In this work,taking Qingdao,China as a typical coastal location,the chemical composition of PM_(2.5)duringwinter 2019was analyzed.Excitation-emission matrix fluorescence spectroscopy was combined with parallel factor analysis model to explain the components of water-soluble atmospheric chromophores of PM_(2.5).Our analysis indicated that NO_(3)^(-),NH_(4)^(+)and SO_(4)^(2-)ions accounted for 86.80%of the total ion mass,dominated by NO_(3)^(-).The ratio of[NO_(3)^(-)]/[SO_(4)^(2-)]was up to 2.42±0.84,suggesting thatmobile sources play an important role in local pollutants emission.The result of positive correlation between Abs_(365)with K^(+)suggests that biomass burning is an important source of water-soluble organic compounds(WSOC).Six types of fluorophores(C1-C6),all humic-like substances,were identified in WSOC.Humification index,biological index and fluorescence index in winter were 1.66±0.34,0.51±0.44 and 1.09±0.78,respectively,indicating that WSOC in Qingdao were mainly terrestrial organic matters.Overall,although the study area is close to the ocean,the contribution of terrestrial sources to PM_(2.5),especially vehicle exhaust and coal combustion,is still much higher than that of marine sources.Our study provides a more comprehensive understanding of chemical and optical properties of WSOC based on PM_(2.5)in coastal areas,and may provide ground for improving local air quality.展开更多
Dissolved organic matter(DOM)in rivers is a critical regulator of the cycling and toxicity of pollutants and the behavior of DOM is a key indicator for the health of the environment.We investigated the sources and cha...Dissolved organic matter(DOM)in rivers is a critical regulator of the cycling and toxicity of pollutants and the behavior of DOM is a key indicator for the health of the environment.We investigated the sources and characteristics of DOM in surface water and sediment samples of the Wei River,China.Dissolved organic carbon(DOC)concentration and ultraviolet absorbance at 254 nm(UV254)increased in the surface water and were decreased in the sediment downstream,indicating that the source of DOM in the water differed from the sediment.Parallel factor(PARAFAC)analysis of the excitation-emission matrices(EEM)revealed the presence of terrestrial humus-like,microbial humus-like and tryptophan-like proteins in the surface water,whereas the sediment contained UVA humic-like,UVC humic-like and fulvic-like in the sediment.The DOM in the surface water and sediment were mainly derived from microbial metabolic activity and the surrounding soil.Surface water DOM displayed greater photodegradation potential than sediment DOM.PARAFAC analysis indicated that the terrestrial humic-like substance in the water and the fulvic-like component in the sediment decomposed more rapidly.These data describe the characteristics of DOM in the Wei River and are crucial to understanding the fluctuations in environmental patterns.展开更多
基金the National Natural Science Foundation of China(No.51778599)the Beijing Natural Science Foundation(No.LI82044)+1 种基金the CAS Strategic Priority Research Programmer(A)(No.XDA20050103)the Youth Innovation Promotion Association CAS(No.110500EA62)。
文摘The membrane bioreactor(MBR)technology is a rising star for wastewater treatment.The pollutant elimination and membrane fouling performances of MBRs are essentially related to the dissolved organic matter(DOM)in the system.Three-dimensional excitation-emission matrix(3D-EEM)fluorescence spectroscopy,a powerful tool for the rapid and sensitive characterization of DOM,has been extensively applied in MBR studies;however,only a limited portion of the EEM fingerprinting information was utilized.This paper revisits the principles and methods of fluorescence EEM,and reviews the recent progress in applying EEM to characterize DOM in MBR studies.We systematically introduced the information extracted from EEM by considering the fluorescence peak location/intensity,wavelength regional distribution,and spectral deconvolution(giving fluorescent component loadings/scores),and discussed how to use the information to interpret the chemical compositions,physiochemical properties,biological activities,membrane retention/fouling behaviors,and migration/transformation fates of DOM in MBR systems.In addition to conventional EEM indicators,novel fluorescent parameters are summarized for potential use,including quantum yield,Stokes shift,excited energy state,and fluorescence lifetime.The current limitations of EEM-based DOM characterization are also discussed,with possible measures proposed to improve applications in MBR monitoring.
基金Supported by the National Natural Science Foundation of China (Grant Nos. 20775025 and 20435010)973 Advanced Research Project (Grant No. 2007CB- 216404)
文摘A novel approach is proposed for direct quantitative analysis of thiabendazole in the orange extract by using excitation-emission matrix fluorescence coupled with second-order calibration methods based on the alternating trilinear decomposition(ATLD) and the alternating normalization-weighted error(ANWE) algorithms,respectively. The average recoveries of thiabendazole in the orange extract by using ATLD and ANWE with an estimated component number of two were 99.7 ± 3.3% and 103.5 ± 4.1%,respectively. Furthermore,the accuracy of the two algorithms was also evaluated through elliptical joint confidence region(EJCR) tests as well as figures of merit,such as sensitivity(SEN),selectivity(SEL) and limit of detection(LOD). The experimental results demonstrate that both algorithms have been satisfactorily applied to the determination of thiabendazole in orange extract,and the perform-ance of ANWE is slightly better than that of ATLD.
基金This study was supported by the Young Beijing Scholars Program and Beijing Agricultural Forestry Academy Foundation(QNJJ202218).
文摘This study established back-propagation neural networks(BPNNs)for evaluating the freshness of bighead carp(Hypophthalmichthys nobilis)heads during chilled storage via fluorescence spectroscopy using an excitation-emission matrix(EEM).The total volatile basic nitrogen(TVB-N)and total aerobic count(TAC)of fish increased obviously during storage at 0,4,8,12,and 16°C,while sensory scores decreased with increasing storage time.The EEM fluorescence intensity was measured,and its change was correlated with the freshness indicators of the samples.Three characteristic components of EEM data were extracted by parallel factor analysis,and two freshness indicators were used to construct the EEM-BPNNs model.The results demonstrated that the relative errors of the EEM-BPNNs model for TVB-N and TAC were less than 14%.This result indicated that the EEM-BPNNs model could determine the freshness of fish in cold chains in a rapid and nondestructive way.
基金funded by the National Natural Science Foundation of China(Grant nos.42276255 and 41976227)project“Impact and Response of Antarctic Seas to Climate Change,IRASCC 2020-2022”(Grant nos.01-01-02A and 02-02-05).
文摘The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to investigate the influence of transparent exopolymer particles(TEP)on the behavior of dissolved organic carbon(DOC)in this region,a comprehensive study was conducted,encompassing both open water areas and highly productive polynyas.It was found that microbial heterotrophic metabolism is the primary process responsible for the production of humic-like fluorescent components in the open ocean.The relationship between apparent oxygen utilization and the two humic-like components can be accurately described by a power-law function,with a conversion rate consistent with that observed globally.The presence of TEP was found to have little impact on this process.Additionally,the study revealed the accumulation of DOC at the sea surface in the Amundsen Sea Polynya,suggesting that TEP may play a critical role in this phenomenon.These findings contribute to a deeper understanding of the dynamics and surface accumulation of DOC in the Amundsen Sea Polynya,and provide valuable insights into the carbon cycle in this region.
基金supported by the National Natural Science Foundation of China(Grant Nos.42130513 and 41625014)the National Key Research and Development Program of China(Grant No.2019YFA0606801)。
文摘To understand the aerosol characteristics in a regional background environment,fine-particle(PM_(2.5),n=228)samples were collected over a one-year period at the Shangdianzi(SDZ)station,which is a Global Atmospheric Watch regional background station in North China.The chemical and optical characteristics of PM_(2.5)were analyzed,including organic carbon,elemental carbon,water-soluble organic carbon,water-soluble inorganic ions,and fluorescent components of watersoluble organic matter.The source factors of major aerosol components are apportioned,and the sources of the fluorescent chromophores are further analyzed.The major chemical components of PM_(2.5)at SDZ were NO_(3)^(-),organic matter,SO_(4)^(2-),and NH_(4)^(+).Annually,water-soluble organic carbon contributed 48%±15%to the total organic carbon.Secondary formation(52%)and fossil fuel combustion(63%)are the largest sources of water-soluble organic matter and water-insoluble organic matter,respectively.In addition,three humic-like and one protein-like matter were identified via parallel factor analysis for excitation–emission matrices.The fluorescence intensities of the components were highest in winter and lowest in summer,indicating the main impact of burning sources.This study contributes to understanding the chemical and optical characteristics of ambient aerosols in the background atmosphere.
基金Supported by the Science and Technology Research Project of Education Department of Hubei Province(Nos.Q20182502,D20152503)the Innovation Team Project of HBNU of Heavy Metal Pollution Mechanism and Ecological Restoration for Lake-Catchment System,Youth Project of Hubei Natural Science Foundation(No.2018CFB321)the Hubei Undergraduate Training Program for Innovation and Entrepreneurship(No.S201910513001)。
文摘Dissolved organic matter(DOM)plays a crucial role in both the carbon cycle and geochemical cycles of other nutrient elements,which is of importance to the management and protection of the aquatic environments.To achieve a more comprehensive understanding the characteristics of DOM in the Changjiang(Yangtze)River basin,water samples from four natural lakes(Xiandao,Baoan,Daye,and Qingshan)in southeastern Hubei Province in China with different eutrophication levels were collected and analyzed.The optical characteristics were analyzed using ultraviolet-visible spectrophotometry and excitation-emission matrix spectroscopy coupled with parallel factor analysis.The results show that:(1)two humic-like components(C1 and C2)and two protein-like substances(C3 and C4)of DOM were identified in all waterbodies;(2)C3 originated primarily from the degradation of microalgae and contributed substantially to humic-like components during transformation.C4 was widely present in the Changjiang River basin and its formation was related to microbial activity,rather than algal blooms or seasons.Influenced by the water mixing,the protein-like components were more likely to be transformed by microorganism,whereas humic-like components were more easily to be photobleached;(3)the concentration of DOM and the fluorescence intensity of humic-like components gradually increased with rising lake eutrophication levels.With respect to protein-like components,only C3 showed changes along the eutrophication gradients;(4)DOM showed a high affinity with permanganate index(COD Mn)and chlorophyll a(chl a)while the relationship was variable with phosphorus.This study helps us systematically understand the DOM characteristics,microbial activities,and pollutant transformation in the Changjiang River basin and provides reference to the ecological restoration of aquatic environments.
基金Under the auspices of the Science and Technology Research Project of Education Department of Hubei Province(No.Q20182502,No.D20152503)Innovation Team Project of HBNU of Heavy Metal Pollution Mechanism and Ecological Restoration for Lake-Catchment System(No.2019CZ014)。
文摘Chromophoric dissolved organic matter(CDOM)is a key component of organic matter that contributes to the ecological functioning of lakes.The lakes in Taihu Lake Basin play an important role in maintaining regional ecological stabilities;however,the optical characteristics of the CDOM in the upstream and downstream lakes in this basin have not yet been systematically studied.Here,the optical characteristics of CDOM in ten lakes of upstream and downstream of the Taihu Lake Basin were studied using UV-Visible and excitation-emission matrix spectroscopies.Three different fluorophores consisting of two humic-like components(C1,C2)and one protein-like component(C3)were identified by parallel factor analysis.Soil or surface erosion was responsible for the higher abund-ance of C1 in the upstream lakes,and increased biological activities accounted for the higher abundance of C3 in the downstream lakes.Rainfall erosion in the wet season led to an increase in CDOM.We also found that the photodegradation and flocculation degree,which played a significant role in reducing CDOM,were higher in downstream lakes than in upstream lakes.Optical analysis of CDOM provides a promising method for monitoring water qualities(e.g.,total phosphorus and potassium permanganate index)in each lake.Re-ductions in soil or surface erosion in the upstream are needed to improve water quality.
基金supported by the German Academic Exchange Service (DAAD)and Higher Education Commission (HEC),Pakistan。
文摘Dissolved organic matter(DOM)in surface waters can vary markedly in character depending on seasonal variations such as rainfall intensity,UV radiations and temperature.Changes in DOM as well as temperature and rainfall intensity over the year can affect the biochemical processes occurring in bank filtration(BF).Identification and characterization of DOM in the surface water could help to optimize the water treatment and provide stable and safe drinking water.This study investigated year-long variations of DOM concentrations and compositions in a surface water of a circulated outdoor pond(research facility)connected to a BF passage.DOM was dominated by humic substances and a changing pattern of DOM in surface water was observed throughout the year.A significant increase of DOM(~38%)in surface water was noted in August compared to November.The fluorescent DOM showed that DOM in summer was enriched with the degradable fraction whilst non-degradable fraction was dominated in winter.A constant(1.7±0.1 mg/L)effluent DOM was recirculated in the system throughout the year.DOM removal through BF varied between 4%to 39%and was achieved within a few meters after infiltration and significantly correlated with influent DOM concentration(R^(2)=0.82,p<0.05).However,no significant(p>0.05)change in the removal of DOM was observed in two subsurface layers(upper and lower).This study highlights the presence of a constant non-degradable DOM in the bank filtrate,which was not affected by temperature,redox conditions and UV radiations.
基金supported by the Second Tibetan Plateau Scientific Expedition and Research Program (STEP,No.2019QZKK0304)the Fundamental Research Funds for the Central Universities (No.E2EG0502×2)the Natural Science Foundation Committee of China (No.41991310)。
文摘Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 vegetable fields in administrative regions of China' Mainland, of which 122 were selected for further investigation. DOM properties were characterized by three-dimensional excitation-emission matrix(3D-EEM) fuorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry(FTICRMS)(field intensity is 15 Tesla). Our results indicated that the main constituents were UVA humic-like substances, humic-like substances, fulvic acid-like substances, and tyrosine-like substances. A total of 10,989 molecular formulae with a mass range of 100.04 to 799.59 Da were detected, covering the mass spectrometric information of the soil samples from 27 different regions. CHO and CHON molecules were dominant in DOM, whereas lignin, tannins,and aromatic substances served as the main components. The results of cluster analysis revealed that the soil properties in Jiangxi Province were considerably different from those in other regions. The key backgrounds of the DOM molecular characteristics in the vegetablefield soil samples across China' Mainland were provided at the molecular level, with large abundance and great variability.
基金supported by the Fundamental Research Funds for the Central Universities (No. E0E48927X2)the National Natural Science Foundation of China (No. 21677145)
文摘Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coexist with Transition Metals(TMs)in PM,have been found to contribute to ROS formation.However,the interaction between WSOCs and TMs and its effect on ROS generation are still unknown.In this study,we examined the ROS concentrations of V,Zn,Suwannee River Fulvic Acid(SRFA),Suwannee River Humic Acid(SRHA)and the mixtures of V/Zn and SRFA/SRHA by using a cell-free 2’,7’-Dichlorodihydrofluorescein(DCFH)assay.The results showed that V or Zn synergistically promoted ROS generated by SRFA,but had an antagonistic effect on ROS generated by SRHA.Fluorescence quenching experiments indicated that V and Zn were more prone to form stable complexes with aromatic humic acid-like component(C1)and fulvic acidlike component(C3)in SRFA and SRHA.Results suggested that the underlying mechanism involving the fulvic acid-like component in SRFA more tending to complex with TMs to facilitate ROS generation throughπelectron transfer.Our work showed that the complexing ability and complexing stability of atmospheric PM organics with metals could significantly affect ROS generation.It is recommended that the research deploying multiple analytical methods to quantify the impact of PM components on public health and environment is needed in the future.
基金supported by the National Natural Science Foundation of China(Nos.41771347 and 4177010514)
文摘Molecular weight(Mw) is a fundamental property of humic acids(HAs), which considerably affect the mobility and speciation of heavy metals in the environment. In this study, soil humic acid(HA) extracted from Jinyun Mountain, Chongqing was ultra-filtered into four fractions according to the molecular weight, and their properties were characterized.Complexation of cadmium was investigated by titration experiments. For the first time,Langmuir and non-ideal competitive adsorption-Donna(NICA-Donnan) models combined with fluorescence excitation-emission matrix(EEM) quenching were employed to elucidate the binding characteristics of individual Mw fractions of HA. The results showed that the concentration of acidic functional groups decreased with increasing Mw, especially the phenolic groups. The humification degree and aliphaticity increased with increasing Mw as indicated by elemental composition analysis and FT-IR spectra. The binding capacity of Cd^(2+) to Mw fractions of HA followed the order UF1(< 5 kDa) > UF2(5–10 kDa) > UF4(> 30 kDa) > UF3(10–30 kDa). Moreover, the distribution of cadmium speciation indicated that the phenolic groups were responsible for the variations in binding of Cd^(2+) among different Mw fractions. The results of fluorescence quenching illustrated that the binding capacity of Cd^(2+) to Mw fractions was controlled by the content of functional groups, while the binding affinity was largely influenced by structural factors. The results provide a better understanding of the roles that different HA Mw fractions play in heavy metal binding,which has important implications in the control of heavy metal migration and bio-toxicity.
基金supported by the National Natural Science Foundation of China(Nos.22076099,21876098,41877354)Youth Innovation Program of Universities in Shandong Province(No.2019KJD007)Fundamental Research Fund of Shandong University(No.2020QNQT012)
文摘Although marine and terrestrial emissions simultaneously affect the formation of atmospheric fine particles in coastal areas,knowledge on the optical properties and sources of water-soluble matter in these areas is still scarce.In this work,taking Qingdao,China as a typical coastal location,the chemical composition of PM_(2.5)duringwinter 2019was analyzed.Excitation-emission matrix fluorescence spectroscopy was combined with parallel factor analysis model to explain the components of water-soluble atmospheric chromophores of PM_(2.5).Our analysis indicated that NO_(3)^(-),NH_(4)^(+)and SO_(4)^(2-)ions accounted for 86.80%of the total ion mass,dominated by NO_(3)^(-).The ratio of[NO_(3)^(-)]/[SO_(4)^(2-)]was up to 2.42±0.84,suggesting thatmobile sources play an important role in local pollutants emission.The result of positive correlation between Abs_(365)with K^(+)suggests that biomass burning is an important source of water-soluble organic compounds(WSOC).Six types of fluorophores(C1-C6),all humic-like substances,were identified in WSOC.Humification index,biological index and fluorescence index in winter were 1.66±0.34,0.51±0.44 and 1.09±0.78,respectively,indicating that WSOC in Qingdao were mainly terrestrial organic matters.Overall,although the study area is close to the ocean,the contribution of terrestrial sources to PM_(2.5),especially vehicle exhaust and coal combustion,is still much higher than that of marine sources.Our study provides a more comprehensive understanding of chemical and optical properties of WSOC based on PM_(2.5)in coastal areas,and may provide ground for improving local air quality.
基金the National Natural Science Foundation of China(Grant No.41977307).
文摘Dissolved organic matter(DOM)in rivers is a critical regulator of the cycling and toxicity of pollutants and the behavior of DOM is a key indicator for the health of the environment.We investigated the sources and characteristics of DOM in surface water and sediment samples of the Wei River,China.Dissolved organic carbon(DOC)concentration and ultraviolet absorbance at 254 nm(UV254)increased in the surface water and were decreased in the sediment downstream,indicating that the source of DOM in the water differed from the sediment.Parallel factor(PARAFAC)analysis of the excitation-emission matrices(EEM)revealed the presence of terrestrial humus-like,microbial humus-like and tryptophan-like proteins in the surface water,whereas the sediment contained UVA humic-like,UVC humic-like and fulvic-like in the sediment.The DOM in the surface water and sediment were mainly derived from microbial metabolic activity and the surrounding soil.Surface water DOM displayed greater photodegradation potential than sediment DOM.PARAFAC analysis indicated that the terrestrial humic-like substance in the water and the fulvic-like component in the sediment decomposed more rapidly.These data describe the characteristics of DOM in the Wei River and are crucial to understanding the fluctuations in environmental patterns.
