Several soil samples were used to study how the characteristics of natural organic matter (NOM) affect sorption of organic compounds. These soils contains different amounts and types of NOM. Aromaticity of NOM (percen...Several soil samples were used to study how the characteristics of natural organic matter (NOM) affect sorption of organic compounds. These soils contains different amounts and types of NOM. Aromaticity of NOM (percentage of aromatic carbons) was determined from solid state CPMAS 13 C NMR spectra and the soil effective polarity was computed from the equation developed by Xing et al . Naphthalene was used to examine the sorption characteristics of NOM. Both aromaticity and polarity of NOM strongly affected sorption of naphthalene. Old NOM showed higher affinity than that in the surface, young soils. Sorption increased with increasing aromaticity and decreasing polarity. Thus, the sorption coefficients of organic contaminants cannot be accurately predicted without some consideration of NOM characteristics.展开更多
In a sanitation process of drinking water, carbon from the organic matter reacts with chlorine, forming by-products, among which are trihalomethanes (THM). These substances are carriers of mutagenic and can-cerogenic ...In a sanitation process of drinking water, carbon from the organic matter reacts with chlorine, forming by-products, among which are trihalomethanes (THM). These substances are carriers of mutagenic and can-cerogenic potential and hence should be removed in drinking water treatment. Since the natural organic mat-ters are precursors of THM formation, their removal from the water decreases the concentration of THMs. The THM forming potential is the most reliable indicator in evaluation of organic matter removal during drinking water treatment processes. The results have shown that the reaction producing THMs follows sec-ond order kinetics. The second order rate constant ranged from 0.024 M-1s-1 to 0.065 M-1s-1 at 22 °C and pH = 8.2 for 96 hours. The removal of 78.4% of natural organic matter, by adsorption on anionic exchange res-ins, resulted in the THM forming potential reduction by 63.1%. Various fractions of natural organic matter differ in their reactivity with chlorine, which is important when it comes to selection of the adsorption me-dium in the drinking water treatment processes.展开更多
Hospital wastewater represents an infectious and toxic risk to human health and the environment due to its contents. Most hospitals in developing countries, including Benin, do not have a wastewater treatment plant. I...Hospital wastewater represents an infectious and toxic risk to human health and the environment due to its contents. Most hospitals in developing countries, including Benin, do not have a wastewater treatment plant. In this study, the wastewater from two hospitals in northern Benin was characterized and then treated with Azadirachta indica leaves, Moringa oleifera and Luffa cylindrica seeds by coagulation/flocculation process. The wastewater characteristics showed that the collected samples are greatly polluted by organic matter and fecal bacteria such as Escherichia coli, Enterococcus fecal and Total coliforms. Jar-test results revealed that 95.74%, 78%, 49.19% of turbidity, 51.35%, 38.32%, 22.19% of COD, 93.16%, 85.26%, 83.30% against Escherichia coli, 92.11%, 90.93%, 94.60% against total Coliforms and 99.37%, 91%, 99%, 55.07% against Enterococcus were removed from hospital wastewater using Moringa oleifera, Luffa cylindrica seed and Azadirachta indica leaves respectively at dose of 100 mg/L. The results highlighted that the natural coagulants could be successfully used for the removal of turbidity and fecal bacteria from hospital wastewater.展开更多
Natural Organic Matter (NOM) is a mixture of aromatic and aliphatic organic compounds of natural origin in any type of aquatic system. Human activities impact the constituents of NOM, from its production to its fate, ...Natural Organic Matter (NOM) is a mixture of aromatic and aliphatic organic compounds of natural origin in any type of aquatic system. Human activities impact the constituents of NOM, from its production to its fate, particularly in the treatment of domestic waste waters. In this work, the impact of microorganisms isolated from a Waste Water Treatment Plant (WWTP) was investigated to determine the fate of NOM fractions in raw sewage, using fluorescence spectroscopy. Wastewater samples were taken at three different times from a WWTP, and incubated for 4 days under two treatments: 1) “raw sewage”, and 2) “spiked”, i.e., the same raw sewage, spiked with bacteria previously isolated from the WWTP. The incubated waters were analyzed by fluorescence spectroscopy, digitally resolved into NOM components: humic- and fulvic-like, and two types of protein-like, i.e., tryptophan- and tyrosine-like, using a Parallel Factor Analysis routine (PARAFAC). The results demonstrate that the “spiked” samples showed the largest changes with incubation time. The signals of the tryptophan- and tyrosine-like components decreased, suggesting a net microbial digestion of proteinaceous material. In contrast, the fulvic-like signals, and to some extent, the humic-like signals increased, suggesting the production of the associated molecular materials during the incubation period. This study provides direct evidence of human impact on the make-up of NOM: the cultures of microbes found at a WWTP consume the proteinaceous material, whereas humic-like and fulvic-like materials are produced.展开更多
The structures of 26 different congeners of polychlorinated biphenyls（PCBs, including monothrough deca-chlorinated） were optimized using density functional theory（DFT） calculations with the 6-31＋G（d,p） basis se...The structures of 26 different congeners of polychlorinated biphenyls（PCBs, including monothrough deca-chlorinated） were optimized using density functional theory（DFT） calculations with the 6-31＋G（d,p） basis set. The activation energies for the dechlorination of these systems were calculated for direct photodegradation and photosensitized degradation reaction pathways in the presence of natural organic matter（NOM）. The dechlorination mechanism of these PCBs and the ring-opening reaction mechanisms（using QST3 method） of the photosensitive degradation products were analyzed. The results showed that（i） the activation energy for the photosensitized degradation of PCBs was much lower than that of direct photodegradation;（ii） the degradation activities（i.e., C–Cl bond cleavage energies） were the same for both degradation pathways and followed the order ortho 〉 meta 〉 para;（iii） the degradation activities of asymmetric PCBs were higher than those of the corresponding symmetrical PCBs for the direct photodegradation and it was completely opposite in the photosensitive degradation;（iv） there was no correlation between the dissociation energy and the number of C–Cl bonds for the direct photodegradation and dechlorination products were all biphenyl;（v） the degradation activity of PCBs decreased as the number of C–Cl bonds increased in the presence of NOM; and（vi） even when the dechlorination reaction was incomplete, it produced chlorophenol. Furthermore, the free radicals of NOM led to the ring-opening reactions of PCBs via an initial addition step. The main site of these ring-opening reactions was the ortho position. Notably, the likelihood of ring-opening reactions occurring involving the degradation products increased as the degradation degree of PCBs increased.展开更多
Ozone plays an important role as a disinfectant and oxidant in potable water treatment practice and is increasingly being used as a pre-oxidant before coagulation. The purpose of this study is to obtain insight into t...Ozone plays an important role as a disinfectant and oxidant in potable water treatment practice and is increasingly being used as a pre-oxidant before coagulation. The purpose of this study is to obtain insight into the mechanisms that are operative in pre-ozonized coagulation. Effects ofpre-ozonation on organic matter removal during coagulation with IPF-PAC1 were investigated by using PDA （photometric disperse analysis）, apparent molecular weight distribution and chemical fractionation. The dynamic formation of flocs during coagulation process was detected. Changes of aquatic organic matter （AOM） structure resulted from the influence of pre-ozonation were evaluated. Results show that dosage of O3 and characteristics of AOM are two of the major factors influencing the performance of O3 on coagulation. No significant coagulation-aid effect of O3 was observed for all experiments using either A1C13 or PAC1. On the contrary, with the application of pre-ozonation, the coagulation efficiency of A1C13 was significantly deteriorated, reflected by the retardation of floc formation, and the removal decreases of turbidity, DOC, and UV254. However, if PACl was used instead of AlCl3, the adverse effects of pre-ozonation were mitigated obviously, particularly when the O3 dosage was less than 0.69 （mg O3/mg TOC）. The difference between removals of UV254, and DOC indicated that pre-ozonation greatly changed the molecular structure of AOM, but its capability of mineralization was not remarkable. Only 5% or so DOC was removed by pre-ozonation at 0.6--0.8 mg/L alone. Fractionation results showed that the organic products of pre-ozonation exhibited lower molecular weight and more hydrophilicity, which impaired the removal of DOC in the following coagulation process.展开更多
Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum...Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum albumin, and different cutoff fractions of natural organic matter(>1 kDa and >3 kDa) obtained from seawater using centrifugal ultrafiltration devices were investigated. For a given element, all the adsorption kinetics did not reach equilibrium except the interaction between Pt and >1 kDa cutoff, and between Pd and humic acid.For all the tested MOCs, the adsorption kinetics could be divided into two stages, a rapid adsorption process in the first 8 h and the desorption stage after the first 8 h until the equilibrium. The change trend of partition coefficient(log10Kd) values with experiment time was consistent with that of the kinetic curves. However, in the interaction between PGE ions and natural dissolved organic matter(NDOM), an obvious difference in the change trends of log10Kd and kinetic curves was observed. It indicated that the partition behavior of PGE ions interacting with NDOM in seawater was a combined effect of different organic constituents. The adsorption and log10Kd of PGEs in the >1 kDa NDOM fraction were higher and more stable than those in the >3 kDa NDOM fraction. The results also indicated that the 1–3 kDa NDOM may dominate the interaction between PGEs ions and NDOM. Moreover, no kinetic model could perfectly simulate the adsorption process. It indicated that the colloidal struction and morphology of MOCs or NDOM in seawater might be inhomogeneous. Hence, the interaction between PGE ions and organic matter in seawater was a complicated process and needs further research.展开更多
Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe R...Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe River sediments sequentially. The results showed that the anaerobic degradation of γ 666, p,p' DDT and HCB followed pseudo first order kinetics in different sediments. But, the extents and rates of degradation were different, even the other conditions remained the same. Anaerobic degradation rates of γ 666, p,p' DDT and HCB were 0 020 d -1 , 0 009 d -1 and 0 035 month -1 respectively for the sediments without additional carbon resources. However, with addition of carbon resources, the anaerobic degradation rates of γ 666, p, p ' DDT and HCB were 0 071 d -1 , 0 054 d -1 and 0 088 month -1 in the original sediments respectively. After removing NOM, the rates were decreased to 0 047 d -1 , 0 037 d -1 and 0 066 month -1 ; in the sediments removed NOM and HMO, the rates were increased to 0 067 d -1 , 0 059 d -1 and 0 086 month -1 . These results indicated that NOM in the sediments accelerated the anaerobic degradation of γ 666, p,p' DDT and HCB; the HMO inhibited the anaerobic degradation of γ 666, p,p' DDT and HCB.展开更多
The application of selenium nanoparticles(SeNPs)as nanofertilizers may lead to the release of SeNPs into aquatic systems.However,the environmental behavior of SeNPs is rarely studied.In this study,using alginate-coate...The application of selenium nanoparticles(SeNPs)as nanofertilizers may lead to the release of SeNPs into aquatic systems.However,the environmental behavior of SeNPs is rarely studied.In this study,using alginate-coated SeNPs(Alg-SeNPs)and polyvinyl alcohol-coated SeNPs(PVA-SeNPs)as models,we systematically investigated the aggregation and stability of SeNPs under various water conditions.PVA-SeNPs were highly stable in mono-and polyvalent electrolytes,probably due to the strong steric hindrance of the capping agent.Alg-SeNPs only suffered from a limited increase in size,even at 2500 mmol/L NaCl and 200 mmol/L MgCl_(2),while they underwent apparent aggregation in CaCl_(2) and LaCl_(3) solutions.The binding of Ca^(2+) and La^(3+) with the guluronic acid part in alginate induced the formation of cross-linking aggregates.Natural organic matter enhanced the stability of Alg-SeNPs in monovalent electrolytes,while accelerated the attachment of Alg-SeNPs in polyvalent electrolytes,due to the cation bridge effects.The long-term stability of SeNPs in natural water showed that the aggregation sizes of Alg-SeNPs and PVA-SeNPs increased to several hundreds of nanometers or above 10μm after 30 days,implying that SeNPs may be suspended in the water column or further settle down,depending on the surrounding water chemistry.The study may contribute to the deep insight into the fate and mobility of SeNPs in the aquatic environment.The varying fate of SeNPs in different natural waters also suggests that the risks of SeNPs to organisms living in diverse depths in the aquatic compartment should be concerned.展开更多
文摘Several soil samples were used to study how the characteristics of natural organic matter (NOM) affect sorption of organic compounds. These soils contains different amounts and types of NOM. Aromaticity of NOM (percentage of aromatic carbons) was determined from solid state CPMAS 13 C NMR spectra and the soil effective polarity was computed from the equation developed by Xing et al . Naphthalene was used to examine the sorption characteristics of NOM. Both aromaticity and polarity of NOM strongly affected sorption of naphthalene. Old NOM showed higher affinity than that in the surface, young soils. Sorption increased with increasing aromaticity and decreasing polarity. Thus, the sorption coefficients of organic contaminants cannot be accurately predicted without some consideration of NOM characteristics.
文摘In a sanitation process of drinking water, carbon from the organic matter reacts with chlorine, forming by-products, among which are trihalomethanes (THM). These substances are carriers of mutagenic and can-cerogenic potential and hence should be removed in drinking water treatment. Since the natural organic mat-ters are precursors of THM formation, their removal from the water decreases the concentration of THMs. The THM forming potential is the most reliable indicator in evaluation of organic matter removal during drinking water treatment processes. The results have shown that the reaction producing THMs follows sec-ond order kinetics. The second order rate constant ranged from 0.024 M-1s-1 to 0.065 M-1s-1 at 22 °C and pH = 8.2 for 96 hours. The removal of 78.4% of natural organic matter, by adsorption on anionic exchange res-ins, resulted in the THM forming potential reduction by 63.1%. Various fractions of natural organic matter differ in their reactivity with chlorine, which is important when it comes to selection of the adsorption me-dium in the drinking water treatment processes.
文摘Hospital wastewater represents an infectious and toxic risk to human health and the environment due to its contents. Most hospitals in developing countries, including Benin, do not have a wastewater treatment plant. In this study, the wastewater from two hospitals in northern Benin was characterized and then treated with Azadirachta indica leaves, Moringa oleifera and Luffa cylindrica seeds by coagulation/flocculation process. The wastewater characteristics showed that the collected samples are greatly polluted by organic matter and fecal bacteria such as Escherichia coli, Enterococcus fecal and Total coliforms. Jar-test results revealed that 95.74%, 78%, 49.19% of turbidity, 51.35%, 38.32%, 22.19% of COD, 93.16%, 85.26%, 83.30% against Escherichia coli, 92.11%, 90.93%, 94.60% against total Coliforms and 99.37%, 91%, 99%, 55.07% against Enterococcus were removed from hospital wastewater using Moringa oleifera, Luffa cylindrica seed and Azadirachta indica leaves respectively at dose of 100 mg/L. The results highlighted that the natural coagulants could be successfully used for the removal of turbidity and fecal bacteria from hospital wastewater.
文摘Natural Organic Matter (NOM) is a mixture of aromatic and aliphatic organic compounds of natural origin in any type of aquatic system. Human activities impact the constituents of NOM, from its production to its fate, particularly in the treatment of domestic waste waters. In this work, the impact of microorganisms isolated from a Waste Water Treatment Plant (WWTP) was investigated to determine the fate of NOM fractions in raw sewage, using fluorescence spectroscopy. Wastewater samples were taken at three different times from a WWTP, and incubated for 4 days under two treatments: 1) “raw sewage”, and 2) “spiked”, i.e., the same raw sewage, spiked with bacteria previously isolated from the WWTP. The incubated waters were analyzed by fluorescence spectroscopy, digitally resolved into NOM components: humic- and fulvic-like, and two types of protein-like, i.e., tryptophan- and tyrosine-like, using a Parallel Factor Analysis routine (PARAFAC). The results demonstrate that the “spiked” samples showed the largest changes with incubation time. The signals of the tryptophan- and tyrosine-like components decreased, suggesting a net microbial digestion of proteinaceous material. In contrast, the fulvic-like signals, and to some extent, the humic-like signals increased, suggesting the production of the associated molecular materials during the incubation period. This study provides direct evidence of human impact on the make-up of NOM: the cultures of microbes found at a WWTP consume the proteinaceous material, whereas humic-like and fulvic-like materials are produced.
基金supported by the Fundamental Research Funds for the Central Universities in 2013(JB2013146)the Key Projects in the National Science&Technology Pillar Program in the Eleventh Five-Year Plan Period(2008BAC43B01)
文摘The structures of 26 different congeners of polychlorinated biphenyls（PCBs, including monothrough deca-chlorinated） were optimized using density functional theory（DFT） calculations with the 6-31＋G（d,p） basis set. The activation energies for the dechlorination of these systems were calculated for direct photodegradation and photosensitized degradation reaction pathways in the presence of natural organic matter（NOM）. The dechlorination mechanism of these PCBs and the ring-opening reaction mechanisms（using QST3 method） of the photosensitive degradation products were analyzed. The results showed that（i） the activation energy for the photosensitized degradation of PCBs was much lower than that of direct photodegradation;（ii） the degradation activities（i.e., C–Cl bond cleavage energies） were the same for both degradation pathways and followed the order ortho 〉 meta 〉 para;（iii） the degradation activities of asymmetric PCBs were higher than those of the corresponding symmetrical PCBs for the direct photodegradation and it was completely opposite in the photosensitive degradation;（iv） there was no correlation between the dissociation energy and the number of C–Cl bonds for the direct photodegradation and dechlorination products were all biphenyl;（v） the degradation activity of PCBs decreased as the number of C–Cl bonds increased in the presence of NOM; and（vi） even when the dechlorination reaction was incomplete, it produced chlorophenol. Furthermore, the free radicals of NOM led to the ring-opening reactions of PCBs via an initial addition step. The main site of these ring-opening reactions was the ortho position. Notably, the likelihood of ring-opening reactions occurring involving the degradation products increased as the degradation degree of PCBs increased.
基金The Hi-Tech Research and Development Program (863) of China (No. 2002AA601120)
文摘Ozone plays an important role as a disinfectant and oxidant in potable water treatment practice and is increasingly being used as a pre-oxidant before coagulation. The purpose of this study is to obtain insight into the mechanisms that are operative in pre-ozonized coagulation. Effects ofpre-ozonation on organic matter removal during coagulation with IPF-PAC1 were investigated by using PDA （photometric disperse analysis）, apparent molecular weight distribution and chemical fractionation. The dynamic formation of flocs during coagulation process was detected. Changes of aquatic organic matter （AOM） structure resulted from the influence of pre-ozonation were evaluated. Results show that dosage of O3 and characteristics of AOM are two of the major factors influencing the performance of O3 on coagulation. No significant coagulation-aid effect of O3 was observed for all experiments using either A1C13 or PAC1. On the contrary, with the application of pre-ozonation, the coagulation efficiency of A1C13 was significantly deteriorated, reflected by the retardation of floc formation, and the removal decreases of turbidity, DOC, and UV254. However, if PACl was used instead of AlCl3, the adverse effects of pre-ozonation were mitigated obviously, particularly when the O3 dosage was less than 0.69 （mg O3/mg TOC）. The difference between removals of UV254, and DOC indicated that pre-ozonation greatly changed the molecular structure of AOM, but its capability of mineralization was not remarkable. Only 5% or so DOC was removed by pre-ozonation at 0.6--0.8 mg/L alone. Fractionation results showed that the organic products of pre-ozonation exhibited lower molecular weight and more hydrophilicity, which impaired the removal of DOC in the following coagulation process.
基金The National Natural Science Foundation of China under contract No.41376083the Strategic Priority Research Program of the Chinese Academy of Sciences under contract No.XDA23050303
文摘Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum albumin, and different cutoff fractions of natural organic matter(>1 kDa and >3 kDa) obtained from seawater using centrifugal ultrafiltration devices were investigated. For a given element, all the adsorption kinetics did not reach equilibrium except the interaction between Pt and >1 kDa cutoff, and between Pd and humic acid.For all the tested MOCs, the adsorption kinetics could be divided into two stages, a rapid adsorption process in the first 8 h and the desorption stage after the first 8 h until the equilibrium. The change trend of partition coefficient(log10Kd) values with experiment time was consistent with that of the kinetic curves. However, in the interaction between PGE ions and natural dissolved organic matter(NDOM), an obvious difference in the change trends of log10Kd and kinetic curves was observed. It indicated that the partition behavior of PGE ions interacting with NDOM in seawater was a combined effect of different organic constituents. The adsorption and log10Kd of PGEs in the >1 kDa NDOM fraction were higher and more stable than those in the >3 kDa NDOM fraction. The results also indicated that the 1–3 kDa NDOM may dominate the interaction between PGEs ions and NDOM. Moreover, no kinetic model could perfectly simulate the adsorption process. It indicated that the colloidal struction and morphology of MOCs or NDOM in seawater might be inhomogeneous. Hence, the interaction between PGE ions and organic matter in seawater was a complicated process and needs further research.
文摘Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe River sediments sequentially. The results showed that the anaerobic degradation of γ 666, p,p' DDT and HCB followed pseudo first order kinetics in different sediments. But, the extents and rates of degradation were different, even the other conditions remained the same. Anaerobic degradation rates of γ 666, p,p' DDT and HCB were 0 020 d -1 , 0 009 d -1 and 0 035 month -1 respectively for the sediments without additional carbon resources. However, with addition of carbon resources, the anaerobic degradation rates of γ 666, p, p ' DDT and HCB were 0 071 d -1 , 0 054 d -1 and 0 088 month -1 in the original sediments respectively. After removing NOM, the rates were decreased to 0 047 d -1 , 0 037 d -1 and 0 066 month -1 ; in the sediments removed NOM and HMO, the rates were increased to 0 067 d -1 , 0 059 d -1 and 0 086 month -1 . These results indicated that NOM in the sediments accelerated the anaerobic degradation of γ 666, p,p' DDT and HCB; the HMO inhibited the anaerobic degradation of γ 666, p,p' DDT and HCB.
基金supported by the National Natural Science Foundation of China(Nos.22076198,42192571,and 21827815).
文摘The application of selenium nanoparticles(SeNPs)as nanofertilizers may lead to the release of SeNPs into aquatic systems.However,the environmental behavior of SeNPs is rarely studied.In this study,using alginate-coated SeNPs(Alg-SeNPs)and polyvinyl alcohol-coated SeNPs(PVA-SeNPs)as models,we systematically investigated the aggregation and stability of SeNPs under various water conditions.PVA-SeNPs were highly stable in mono-and polyvalent electrolytes,probably due to the strong steric hindrance of the capping agent.Alg-SeNPs only suffered from a limited increase in size,even at 2500 mmol/L NaCl and 200 mmol/L MgCl_(2),while they underwent apparent aggregation in CaCl_(2) and LaCl_(3) solutions.The binding of Ca^(2+) and La^(3+) with the guluronic acid part in alginate induced the formation of cross-linking aggregates.Natural organic matter enhanced the stability of Alg-SeNPs in monovalent electrolytes,while accelerated the attachment of Alg-SeNPs in polyvalent electrolytes,due to the cation bridge effects.The long-term stability of SeNPs in natural water showed that the aggregation sizes of Alg-SeNPs and PVA-SeNPs increased to several hundreds of nanometers or above 10μm after 30 days,implying that SeNPs may be suspended in the water column or further settle down,depending on the surrounding water chemistry.The study may contribute to the deep insight into the fate and mobility of SeNPs in the aquatic environment.The varying fate of SeNPs in different natural waters also suggests that the risks of SeNPs to organisms living in diverse depths in the aquatic compartment should be concerned.
