Simulated photo-degradation of fluorescent dissolved organic matter(FDOM) in Lake Baihua(BH) and Lake Hongfeng(HF) was investigated with three-dimensional excitationemission matrix(3 DEEM) fluorescence combined with t...Simulated photo-degradation of fluorescent dissolved organic matter(FDOM) in Lake Baihua(BH) and Lake Hongfeng(HF) was investigated with three-dimensional excitationemission matrix(3 DEEM) fluorescence combined with the fluorescence regional integration(FRI),parallel factor(PARAFAC) analysis,and multi-order kinetic models.In the FRI analysis,fulvic-like and humic-like materials were the main constituents for both BH-FDOM and HF-FDOM.Four individual components were identified by use of PARAFAC analysis as humic-like components(C1),fulvic-like components(C2),protein-like components(C3) and unidentified components(C4).The maximum 3 DEEM fluorescence intensity of PARAFAC components C1-C3 decreased by about 60%,70% and 90%,respectively after photo-degradation.The multi-order kinetic model was acceptable to represent the photo-degradation of FDOM with correlation coefficient(Radj2)(0.963-0.998).The photo-degradation rate constants(kn) showed differences of three orders of magnitude,from 1.09 × 10-6 to 4.02 × 10-4 min-1,and half-life of multi-order model(T1/2n)ranged from 5.26 to 64.01 min.The decreased values of fluorescence index(FI) and biogenic index(BI),the fact that of percent fluorescence response parameter of Region I(PⅠ,n) showed the greatest change ratio,followed by percent fluorescence response parameter of Region II(PⅡ,n,while the largest decrease ratio was found for C3 components,and the lowest T1/2n was observed for C3,indicated preferential degradation of protein-like materials/components derived from biological sources during photodegradation.This research on the degradation of FDOM by 3 DEEM/FRI-PARAFAC would be beneficial to understanding the photo-degradation of FD OM in natural environments and accurately predicting the environmental behaviors of contaminants in the presence of FDOM.展开更多
The behavior of pesticide in soil is influenced by dissolved organic matter(DOM)through competition adsorption,adsorption,solubilization,accelerated degradation,and so on.Thus DOM and its components play an important ...The behavior of pesticide in soil is influenced by dissolved organic matter(DOM)through competition adsorption,adsorption,solubilization,accelerated degradation,and so on.Thus DOM and its components play an important role in the environmental risk in the soil ecosystem and groundwater environment.Currently,most studies focused on the short-term effect of high concentration of DOM on the pesticide residues.However,soil DOM is mainly at low level.Therefore,there is of some practical significance to probe into the environmental behavior of soil pesticides under natural level of DOM.Thus a site investigation was conducted in the farmland with long-term application history of pesticide.By using the three dimensional excitation-emission fluorescence matrix(3D-EEM)technology,together with the fluorescence regional integration(FRI)quantitative method,the long-term effects of pesticide residues under low concentration of natural DOM were analyzed.Results showed that:(1)The long-term effects of the natural DOM components on the environment behavior of most soil organo-chlorine pesticides were not significant except for a few pesticides such asγ-HCH,p,p'-DDE,etc.(2)The influencing effects of DOM components on different type of pesticides were varied.Among which,the content of tyrosine component showed a significantly negative correlation(p〈0.05)with the concentration ofγ-HCH and p,p'-DDE.There were significant positive correlations(p〈0.05)between the by-products of microbial degradation in DOM components and the concentration of heptachlor.There were also a significant positive correlation(p〈0.05)between the content of active humus component of humic acid in the DOM and the concentration of heptachlor epoxide.These results suggested that the distribution of different types of pesticides residue in the soil was influenced by different components at different levels of significance.(3)The humification degree of soil organic matter showed minor effect of DOM on the pesticide residues in the soil.In this study,3D-EEM and FRI technology were firstly coupled in use for studying the influence of different components of DOM in soil on the environmental behavior of pesticides,which provides a new idea for the research on the mechanism of pesticides transportation and transformation in soil and groundwater environment.展开更多
In this study, a magnetic micro-particle conditioning–pressurized vertical electro-osmotic dewatering（MPEOD） process with magnetic micro-particle conditioning–drainage under gravity–mechanical compression–electr...In this study, a magnetic micro-particle conditioning–pressurized vertical electro-osmotic dewatering（MPEOD） process with magnetic micro-particle conditioning–drainage under gravity–mechanical compression–electrical compression（MMPC–DG–MC–EC） stages was established to study the distribution and migration of water, extracellular polymeric substances（EPS）, and other organic matter in the activated sludge（AS） matrix at each stage.Results showed that the MPEOD process could attain 53.52% water content（WC） in dewatered AS with bound water（BW） and free water（FW） reduction rates of 82.97% and 99.67%,respectively. The coagulation and time-delayed magnetic field effects of magnetic microparticles（MMPs） along the MMPC–DG–MC stages initiated the transformation of partial BW to FW in AS. EC had a coupling driving effect of electro-osmosis and pressure on BW, and the changes in pH and temperature at EC stage induced the aggregation of AS flocs and the release of partial BW. Additionally, MMPs dosing further improved the dewatering performance of AS by acting as skeleton builders to provide water passages. Meanwhile, MMPs could disintegrate sludge cells and EPS fractions, thereby reducing tryptophan-like protein and byproduct-like material concentrations in LB-EPS as well as protein/polysaccharide ratio in AS matrix, which could improve AS filterability. At EC stage, the former four Ex/Em regions of fluorescence regional integration analysis for EPS were obviously reduced, especially the protein-like substances in LB-and TB-EPS, which contributed to improvement of AS dewaterability.展开更多
The quantification and effects of system pH value on the interactions between Pb（II） and the biopolymer in activated sludge were investigated. The biopolymer had two protein-like fluorescence peaks （Ex/Em = 280 nm1...The quantification and effects of system pH value on the interactions between Pb（II） and the biopolymer in activated sludge were investigated. The biopolymer had two protein-like fluorescence peaks （Ex/Em = 280 nm1326-338 nm for peak A; Ex/Em = 220-230 nm/324-338 nm for peak B）. The fluorescence intensities of peak B were higher than those of peak A. The fluorophores of both peaks could be largely quenched by Pb（ll）, and the quencher dose for peak B was about half of that for peak A. The modified Stern-Volmer equation well depicted the fluorescence quenching titration. The quenching constant （Ka） values for both peaks decreased with rising system pH value, and then sharply decreased under alkaline conditions. It could be attributed to that the alkaline conditions caused the reduction of available Pb（II） due to the occurrence of Pb（OH）2 sediments. The Ka values of peak B were bigger than those for peak A at the same system pH values. Accordingly, the aromatic proteins （peak B） played a key role in the interactions between metal ions and the biopolymer.展开更多
基金financially supported by the National Natural Science Foundation of China(No.41573130)BNU Interdisciplinary Research Foundation for First-Year Doctoral Candidates(No.BNUXKJC1802)
文摘Simulated photo-degradation of fluorescent dissolved organic matter(FDOM) in Lake Baihua(BH) and Lake Hongfeng(HF) was investigated with three-dimensional excitationemission matrix(3 DEEM) fluorescence combined with the fluorescence regional integration(FRI),parallel factor(PARAFAC) analysis,and multi-order kinetic models.In the FRI analysis,fulvic-like and humic-like materials were the main constituents for both BH-FDOM and HF-FDOM.Four individual components were identified by use of PARAFAC analysis as humic-like components(C1),fulvic-like components(C2),protein-like components(C3) and unidentified components(C4).The maximum 3 DEEM fluorescence intensity of PARAFAC components C1-C3 decreased by about 60%,70% and 90%,respectively after photo-degradation.The multi-order kinetic model was acceptable to represent the photo-degradation of FDOM with correlation coefficient(Radj2)(0.963-0.998).The photo-degradation rate constants(kn) showed differences of three orders of magnitude,from 1.09 × 10-6 to 4.02 × 10-4 min-1,and half-life of multi-order model(T1/2n)ranged from 5.26 to 64.01 min.The decreased values of fluorescence index(FI) and biogenic index(BI),the fact that of percent fluorescence response parameter of Region I(PⅠ,n) showed the greatest change ratio,followed by percent fluorescence response parameter of Region II(PⅡ,n,while the largest decrease ratio was found for C3 components,and the lowest T1/2n was observed for C3,indicated preferential degradation of protein-like materials/components derived from biological sources during photodegradation.This research on the degradation of FDOM by 3 DEEM/FRI-PARAFAC would be beneficial to understanding the photo-degradation of FD OM in natural environments and accurately predicting the environmental behaviors of contaminants in the presence of FDOM.
基金National Science&Technology Pillar Program during the 12th Five-year Plan Period(2012BAC19B03)National Natural Science Fund(41271236)+2 种基金Ministry of water resources“948”project(201328)National Public Benefit(Ministry of water resources)Research Foundation(201301039)Science Foundation for Young Scholars North China University of Water Resources and Electric Power(70459)
文摘The behavior of pesticide in soil is influenced by dissolved organic matter(DOM)through competition adsorption,adsorption,solubilization,accelerated degradation,and so on.Thus DOM and its components play an important role in the environmental risk in the soil ecosystem and groundwater environment.Currently,most studies focused on the short-term effect of high concentration of DOM on the pesticide residues.However,soil DOM is mainly at low level.Therefore,there is of some practical significance to probe into the environmental behavior of soil pesticides under natural level of DOM.Thus a site investigation was conducted in the farmland with long-term application history of pesticide.By using the three dimensional excitation-emission fluorescence matrix(3D-EEM)technology,together with the fluorescence regional integration(FRI)quantitative method,the long-term effects of pesticide residues under low concentration of natural DOM were analyzed.Results showed that:(1)The long-term effects of the natural DOM components on the environment behavior of most soil organo-chlorine pesticides were not significant except for a few pesticides such asγ-HCH,p,p'-DDE,etc.(2)The influencing effects of DOM components on different type of pesticides were varied.Among which,the content of tyrosine component showed a significantly negative correlation(p〈0.05)with the concentration ofγ-HCH and p,p'-DDE.There were significant positive correlations(p〈0.05)between the by-products of microbial degradation in DOM components and the concentration of heptachlor.There were also a significant positive correlation(p〈0.05)between the content of active humus component of humic acid in the DOM and the concentration of heptachlor epoxide.These results suggested that the distribution of different types of pesticides residue in the soil was influenced by different components at different levels of significance.(3)The humification degree of soil organic matter showed minor effect of DOM on the pesticide residues in the soil.In this study,3D-EEM and FRI technology were firstly coupled in use for studying the influence of different components of DOM in soil on the environmental behavior of pesticides,which provides a new idea for the research on the mechanism of pesticides transportation and transformation in soil and groundwater environment.
基金supported by the National Natural Science Foundation of China(Nos.51478041,51678053)Major Projects on Control and Rectification of Water Body Pollution(Nos.2012ZX07105-002-03,2013ZX07202-010)
文摘In this study, a magnetic micro-particle conditioning–pressurized vertical electro-osmotic dewatering（MPEOD） process with magnetic micro-particle conditioning–drainage under gravity–mechanical compression–electrical compression（MMPC–DG–MC–EC） stages was established to study the distribution and migration of water, extracellular polymeric substances（EPS）, and other organic matter in the activated sludge（AS） matrix at each stage.Results showed that the MPEOD process could attain 53.52% water content（WC） in dewatered AS with bound water（BW） and free water（FW） reduction rates of 82.97% and 99.67%,respectively. The coagulation and time-delayed magnetic field effects of magnetic microparticles（MMPs） along the MMPC–DG–MC stages initiated the transformation of partial BW to FW in AS. EC had a coupling driving effect of electro-osmosis and pressure on BW, and the changes in pH and temperature at EC stage induced the aggregation of AS flocs and the release of partial BW. Additionally, MMPs dosing further improved the dewatering performance of AS by acting as skeleton builders to provide water passages. Meanwhile, MMPs could disintegrate sludge cells and EPS fractions, thereby reducing tryptophan-like protein and byproduct-like material concentrations in LB-EPS as well as protein/polysaccharide ratio in AS matrix, which could improve AS filterability. At EC stage, the former four Ex/Em regions of fluorescence regional integration analysis for EPS were obviously reduced, especially the protein-like substances in LB-and TB-EPS, which contributed to improvement of AS dewaterability.
基金Acknowledgements This work was supported by the Foundation of State Key Laboratory of Pollution Control and Resource Reuse （Tongji University）, China （No. PCRRE16019）, the National Natural Science Foundation of China （Grant Nos. 51678422 and 51378368）, Sheng Yun- Fei College Students Scientific and Technological Innovation Fund, China Scholarship Council （No. 201506260022）, the National Science ＆ Technology Pillar Program （No. 2013BAD21B03）, and the higher school innovative engineering plan （111 Projec0.
文摘The quantification and effects of system pH value on the interactions between Pb（II） and the biopolymer in activated sludge were investigated. The biopolymer had two protein-like fluorescence peaks （Ex/Em = 280 nm1326-338 nm for peak A; Ex/Em = 220-230 nm/324-338 nm for peak B）. The fluorescence intensities of peak B were higher than those of peak A. The fluorophores of both peaks could be largely quenched by Pb（ll）, and the quencher dose for peak B was about half of that for peak A. The modified Stern-Volmer equation well depicted the fluorescence quenching titration. The quenching constant （Ka） values for both peaks decreased with rising system pH value, and then sharply decreased under alkaline conditions. It could be attributed to that the alkaline conditions caused the reduction of available Pb（II） due to the occurrence of Pb（OH）2 sediments. The Ka values of peak B were bigger than those for peak A at the same system pH values. Accordingly, the aromatic proteins （peak B） played a key role in the interactions between metal ions and the biopolymer.
