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1.
Zuehlke S  Duennbier U  Heberer T 《Chemosphere》2007,69(11):1673-1680
Residues of phenazone-type pharmaceuticals originating from spills of a former pharmaceutical production plant have recently been detected in ground water in Berlin, Germany. The degradation pathways of phenazone, propyphenazone, and dimethylaminophenazone (DMAA) during water purification were enlightened in batch experiments with groundwater and filter material obtained from operating waterworks. For phenazone and propyphenazone a complete biological transformation into their respective metabolites 1,5-dimethyl-1,2-dehydro-3-pyrazolone (DP) and 4-(2-methylethyl)-1,5-dimethyl-1,2-dehydro-3-pyrazolone (PDP) was observed. Generally, removal of phenazone-type pharmaceutical residues during rapid sand filtration was almost exclusively caused by microorganisms only present in polluted raw water. DMAA applied to fresh filter materials was rapidly degraded into its metabolites 1-acetyl-1-methyl-2-phenylhydrazide (AMPH), acetoaminoantipyrine (AAA), formylaminoantipyrine (FAA), and 1-acetyl-1-methyl-2-dimethyloxamoyl-2-phenylhydrazide (AMDOPH). DMAA, AAA, and FAA were, however, only detected at low levels in a few samples of purified water from an operating water works. Whereas, the metabolites AMDOPH and DP were detected up to 1 microg l(-1). Propyphenazone was rapidly removed and AMPH, phenazone, and PDP were only measured with concentrations in the low ng l(-1) range. The concentrations of the metabolites DP and PDP are even higher in the purified water than in the raw water caused by their formation during degradation of phenazone and propyphenazone. Reduction of filtration velocity on an experimental filter from 5 m h(-1) down to 2 m h(-1) resulted in improved removal of phenazone, propyphenazone and their metabolites DP and PDP, respectively. AMDOPH, however, was highly persistent in all experiments independent from filtration velocities and contact times.  相似文献   

2.
The behaviour of residues of phenazone-type pharmaceuticals during bank filtration was investigated at a field site in Berlin, Germany, where bank-filtered water is used for drinking water production. The concentrations of the pharmaceutical residues in the shallow, young bank filtrate (travel times相似文献   

3.
Residues of three phenazone-type pharmaceuticals have been identified in routine analyses of groundwater samples from selected areas in the north-western districts of Berlin, Germany. Phenazone, propiphenazone, and dimethylaminophenazone have been detected in some wells at concentrations up to the low microg/l-level. Additionally, three phenazone-type metabolites namely 1-acetyl-1-methyl-2-dimethyl-oxamoyl-2-phenylhydrazide (AMDOPH), 1-acetyl-1-methyl-2-phenylhydrazide, and dimethyloxalamide acid-(N'-methyl-N-phenyl)-hydrazide have also been identified in these groundwater samples. The residues are suspected to originate from former production spills of a pharmaceutical plant located in a city north of Berlin. It was observed that with the exception of AMDOPH all other residues were efficiently removed during conventional drinking water treatment. The drug metabolite AMDOPH deriving from dimethylaminophenazone residues was found at concentrations of 0.9 microg/l in finished drinking water. However, a following study on the toxicological relevance of the AMDOPH residues has shown that there is no toxicological harm for humans at the low concentrations of AMDOPH observed in Berlin drinking water.  相似文献   

4.
A water surface sampler (WSS) was employed in combination with greased knife-edge surface deposition plates (KSSs) to measure the vapor phase deposition rates of PCBs to the sampler at an urban site, Chicago, IL. This sampler employed a water circulation system that continuously removed deposited PCBs. Total (gas+particle) and particulate PCB fluxes were collected with the WSS and KSSs, respectively. Gas phase PCB fluxes were then calculated by subtracting the KSS fluxes (particulate) from the WSS fluxes (gas+particle). The calculated gas phase PCB fluxes averaged 830±910 ng m−2d−1. This flux value is, in general, higher than the fluxes determined using simultaneously measured air–water concentrations in natural waters and is in the absorption direction. This difference is primarily because the PCBs were continuously removed from the WSS water keeping the water PCB concentration near zero.Concurrently, ambient air samples were collected using a modified high volume air sampler. The gas phase PCB concentrations ranged between 1.10 and 4.46 ng m−3 (average±SD, 2.29±1.28 ng m−3). The gas phase fluxes were divided by the simultaneously measured gas phase ambient concentrations to determine the overall gas phase mass transfer coefficients (MTCs) for PCBs. The average gas phase overall MTCs (Kg) for each homolog group ranged between 0.22 and 1.32 cm s−1 (0.54±0.47 cm s−1). The average MTC was in good agreement with those determined using similar techniques.  相似文献   

5.
《Chemosphere》2013,90(11):1307-1315
This study investigated the presence and distribution of 22 antibiotics, including eight quinolones, nine sulfonamides and five macrolides, in the water, sediments, and biota samples from Baiyangdian Lake, China. A total of 132 samples were collected in 2008 and 2010, and laboratory analyses revealed that antibiotics were widely distributed in the lake. Sulfonamides were the dominant antibiotics in the water (0.86–1563 ng L−1), while quinolones were prominent in sediments (65.5–1166 μg kg−1) and aquatic plants (8.37–6532 μg kg−1). Quinolones (17.8–167 μg kg−1) and macrolides [from below detection limit (BDL) to 182 μg kg−1] were often found in aquatic animals and birds. Salvinia natans exhibited the highest bioaccumulation capability for quinolones among three species of aquatic plants. Geographical differences of antibiotic concentrations were greatly due to anthropogenic activities. Sewage discharged from Baoding City was likely the main source of antibiotics in the lake. Risk assessment of antibiotics on aquatic organisms suggested that algae and aquatic plants might be at risk in surface water, while animals were likely not at risk.  相似文献   

6.
Carbonyl compounds exist in the atmosphere as either gases or aerosols. Some of them are water soluble and known as oxidation products of biogenic and/or anthropogenic hydrocarbons. Five carbonyl compounds, glyoxal (GO), 4-oxopentanal (4-OPA), glycolaldehyde (GA), hydroxyacetone (HA) and methylglyoxal (MG) have been identified in a temporal series of 12 rain samples. The concentrations of the compounds in the samples were high at the beginning of the rain event and decreased with time to relatively low and fairly constant levels, indicating that the compounds were washed out from the atmosphere at the start of the rain event. Possibly, these compounds also existed in the cloud condensation nuclei (CCN). Wet deposition rates of the carbonyl compounds were calculated for nine samples collected during a 20 h period. The deposition rates ranged from 0 (4-OPA) to 1.2×10−1 mg C m−2 h−1 (MG) with the average of 2.9×10−2 mg C m−2 h−1. Production rates of isoprene oxidation products (GA, HA and MG) in the area surrounding the sampling site were estimated with a chemical box model. The deposition rates exceeded the production rates in most samples. This indicates that the rainfall causes a large net flux of the water soluble compounds from the atmosphere to the ground. Insoluble carbonyl compounds such as n-nonanal and n-decanal were expected to be present in the atmosphere, but were not detected in the rain during the sampling period, suggesting that an aerosol containing these insoluble compounds does not effectively act as a CCN.  相似文献   

7.
Real-world vehicle emissions of carbonyls were determined in summer and winter of 2003 at the Shing Mun Tunnel, Hong Kong. Fifteen carbonyl species have been analyzed in this study. The total measured carbonyls emission factors ranged from 21.7 to 68.9 mg veh−1 km−1 among different measurement periods, with an average of 35.8±11.9 mg veh−1 km−1. Higher carbonyl emissions were found to be associated with a high proportion of diesel-fueled vehicles. Total measured carbonyl emissions from Diesel-fueled Vehicle (DV, 71.5 mg veh−1 km−1) were about 7 times higher than those from Non-Diesel-fueled Vehicle (NDV, 10 mg veh−1 km−1). The five carbonyls with the largest DV emission factor were, in decreasing order, formaldehyde (38.3 mg veh−1 km−1), acetaldehyde (11.4 mg veh−1 km−1), acetone (5.3 mg veh−1 km−1), crotonaldehyde (5.2 mg veh−1 km−1) and benzaldehyde (2.0 mg veh−1 km−1). These five carbonyl compounds together accounted for 87% of the sum of all DV carbonyl emission factors. For NDV, the five most abundant carbonyls in NDV emission at the tunnel were, in decreasing order, formaldehyde (3.5 mg veh−1 km−1), acetone (1.8 mg veh−1 km−1), methyl ethyl ketone (1.6 mg veh−1 km−1), m,p-tolualdehyde (1.0 mg veh−1 km−1) and acetaldehyde (mg veh−1 km−1). They accounted for 85% of the sum of all NDV carbonyl emission factors.  相似文献   

8.
Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m−3 in air samples and from 50 to 312 ng l−1 in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m −3) compared to the summer and winter (37–161 ng m−3). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m− 2 yr− 1), relative to wet deposition (130 μg m−2 yr− 1) and dry deposition (99 μg m−2 yr− 1). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr−1.  相似文献   

9.
《Chemosphere》2013,90(11):1414-1418
Nano-MgO is a good bactericide but with strong alkalinity in water due to its rapid hydrolysis. To control its hydrolysis rate and keep its bactericidal properties, we synthesized nano-MgO microspheres using chitosan–alginate system in this study. The synthesized nano-MgO release-controlled microspheres (nMgO-RCM) were with 0.98–1.20 mm of particle sizes. Also, their embedding ratio and loading percentage was 63.52% and 12.27%, respectively. Based on the characterization results, nano-MgO was only observed on surface of the nMgO-RCM. Its release rate from the nMgO-RCM could be controlled by the chitosan–alginate system, and the observed rate constant (kobs) increased from 0.0289 h−1 to 0.0358 h−1 with the increment of the dosage from 10 mg L−1 to 80 mg L−1. Furthermore, the nMgO-RCM could maintain pH value lower than 8.5 and colony counts less than 20 CFU mL−1 for at least 120 h.  相似文献   

10.
Due to the high temporal and spatial variability of N2O fluxes, estimates of N2O emission from temperate forest ecosystems are still highly uncertain, particularly at larger scales. Although highest N2O emissions with up to 7.0 kg N ha−1 yr−1 were mainly reported for soils affected by stagnant water, most of the reported gas flux measurements were performed at forest sites with well-aerated soils yielding mostly to low mean annual emission rates less than 1.0 kg N ha−1 yr−1. This study compares N2O fluxes from upland (Cambisols) and temporally water-logged (Gleysols, Histosols) soils of the Central Black Forest (South-West Germany) over a period of 2 yr. Mean annual N2O fluxes from investigated soils ranged between 0.2 and 3.9 kg N ha−1 yr−1. The fluxes showed a large variability between the different soil types. Emissions could be clearly ranked in the following order: Cambisols (0.26–0.75 kg N ha−1 yr−1)<Gleysols (1.37–2.68 kg N ha−1 yr−1)<Histosol (3.66–3.95 kg N ha−1 yr−1). Although the Cambisols cover two-thirds of the investigated area, only about half of the overall N2O is emitted from this soil type. Therefore, regional or national N2O fluxes from temperate forest soils are underestimated if soils characterised by intermediate aeration conditions are disregarded.  相似文献   

11.
Ammonia-nitrogen flux (NH3-N=(14/17)NH3) was determined from six anaerobic swine waste storage and treatment lagoons (primary, secondary, and tertiary) using the dynamic chamber system. Measurements occurred during the fall of 1998 through the early spring of 1999, and each lagoon was examined for approximately one week. Analysis of flux variation was made with respect to lagoon surface water temperature (∼15 cm below the surface), lagoon water pH, total aqueous phase NHx(=NH3+NH4+) concentration, and total Kjeldahl nitrogen (TKN). Average lagoon temperatures (across all six lagoons) ranged from approximately 10.3 to 23.3°C. The pH ranged in value from 6.8 to 8.1. Aqueous NHx concentration ranged from 37 to 909 mg N l−1, and TKN varied from 87 to 950 mg N l−1. Fluxes were the largest at the primary lagoon in Kenansville, NC (March 1999) with an average value of 120.3 μg N m−2 min−1, and smallest at the tertiary lagoon in Rocky Mount, NC (November 1998) at 40.7 μg N m−2 min−1. Emission rates were found to be correlated with both surface lagoon water temperature and aqueous NHx concentration. The NH3-N flux may be modeled as ln(NH3-N flux)=1.0788+0.0406TL+0.0015([NHx]) (R2=0.74), where NH3-N flux is the ammonia flux from the lagoon surface in μg N m−2 min−1, TL is the lagoon surface water temperature in °C, and [NHx] is the total ammonia-nitrogen concentration in mg N l−1.  相似文献   

12.
To evaluate the tropical wetlands contribution to the methane (CH4) burden better, field campaigns were performed during 2004 and 2005 near the Miranda River, in five sites inside the Brazilian Pantanal region. The CH4 fluxes were determined using the static chamber technique. Environmental variables that may affect CH4 emissions, as the water depth, the water and air temperatures were also measured. The overall average of the 320 individual CH4 flux measurements made between March/2004 and March/2005 was 142±314 mg CH4 m−2 d−1, which is a value near the ones observed in other tropical flooded regions. About 47% of the fluxes measurements presented nonlinear increases in the chamber concentrations, which were assumed to be linked to CH4 losses through bubbles. The bubble flux represented about 90% of the total CH4 losses in the measurements and ranged from 1 to 2187 mg CH4 m−2 d−1 with an average of 292±410 mg CH4 m−2 d−1 (median: 153 mg CH4 m−2 d−1). The diffusive flux ranged from 1 to 124 mg CH4 m−2 d−1, with an average of 10±17 mg CH4 m−2 d−1 (median: 5 mg CH4 m−2 d−1). The fluxes from lakes were smaller than those observed in the floodplains, where the flooding was more dependent on the seasonal cycle. The diffusive flux showed a slight, but not statistically significant seasonal variation, following the seasonal variation of the flooding of the Pantanal region. A rough estimative of the total annual CH4 emission shows that the contribution of the Pantanal is about 3.3 Tg CH4 yr−1, which represents about 3.3% of the total CH4 emissions estimated to be originated in wetlands ecosystems. It may be a conservative estimate, which may present a large interannual variation, since it was obtained during one of the lowest flood of the Pantanal in recent years.  相似文献   

13.
Gaseous methane (CH4) emissions from a swine waste holding lagoon were determined periodically during the year. Micrometeorological techniques were used in order that emission rates from the lagoon were measured under ambient conditions with little disturbance to the natural environment. During the cold winter measurement period, CH4 fluxes were linearly related to lagoon water temperature below 22°C (r=0.87). During warmer measurement periods, both water and air temperatures and windspeed affected emissions rates. In general, flux rates followed a diurnal pattern with greater fluxes during the day when both temperature and windspeed were greatest. Mathematical models using air and water temperature and windspeed factors could explain 47 to 75% of the variation in fluxes. Daily emission rates ranged from 1 to 500 kg CH4 ha−1 d−1. The average flux for the year was 52.3 kg CH4 ha−1 d−1 which corresponded to about 5.6 kg CH4 animal−1 yr−1 from the primary lagoon.  相似文献   

14.
Emissions of nitric oxide (NO) were determined during late spring and summer 1995 and the spring of 1996 from four agricultural soils on which four different crops were grown. These agricultural soils were located at four different sites throughout North Carolina. Emission rates were calculated using a dynamic flow-through chamber system coupled to a mobile laboratory for in-situ analysis. Average NO fluxes during late spring 1995 were: 50.9±47.7 ng N m−2 s−1 from soil planted with corn in the lower coastal plain. Average NO fluxes during summer 1995 were: 6.4±4.6 and 20.2±19.0 ng N m−2 s−1, respectively, from soils planted with corn and soybean in the coastal region; 4.2±1.7 ng N m−2 s−1 from soils planted with tobacco in the piedmont region; and 8.5±4.9 ng N m−2 s−1 from soils planted with corn in the upper piedmont region. Average NO fluxes for spring 1996 were: 66.7±60.7 ng N m−2 s−1 from soils planted with wheat in the lower coastal plain; 9.5±2.9 ng N m−2 s−1 from soils planted with wheat in the coastal plain; 2.7±3.4 ng N m−2 s−1 from soils planted with wheat in the piedmont region; and 56.1±53.7 ng N m−2 s−1 from soils planted with corn in the upper piedmont region. An apparent increase in NO flux with soil temperature was present at all of the locations. The composite data from all the research sites revealed a general positive trend of increasing NO flux with soil water content. In general, increases in total extractable nitrogen (TEN) appeared to be related to increased NO emissions within each site, however a consistent trend was not evident across all sites.  相似文献   

15.
The quality of an emission calculation model based on emission factors measured on roller test stands and statistical traffic data was evaluated using source strengths and emission factors calculated from real-world exhaust gas concentration differences measured upwind and downwind of a motorway in southwest Germany. Gaseous and particulate emissions were taken into account. Detailed traffic census data were taken during the measurements. The results were compared with findings of similar studies.The main conclusion is the underestimation of CO and NOx source strengths by the model. On the average, it amounts to 23% in case of CO and 17% for NOx. The latter underestimation results from an undervaluation by 22% of NOx emission factors of heavy-duty vehicles (HDVs). There are significant differences between source strengths on working days and weekends because of the different traffic split between light-duty vehicles (LDVs) and HDVs. The mean emission factors of all vehicles from measurements are 1.08 g km−1 veh−1 for NOx and 2.62 g km−1 veh−1 for CO. The model calculations give 0.92 g km−1 veh−1 for NOx and 2.14 g km−1 veh−1 for CO.The source strengths of 21 non-methane hydrocarbon (NMHC) compounds quantified are underestimated by the model. The ratio between the measured and model-calculated emissions ranges from 1.3 to 2.1 for BTX and up to 21 for 16 other NMHCs. The reason for the differences is the insufficient knowledge of NMHC emissions of road traffic.Particulate matter emissions are dominated by ultra-fine particles in the 10–40 nm range. As far as aerosols larger than 29 nm are concerned, 1.80×1014 particles km−1 veh−1 are determined for all vehicles, 1.22×1014 particles km−1 veh−1 and an aerosol volume of 0.03 cm3 km−1 veh−1 are measured for LDVs, and for HDVs 7.79×1014 particles km−1 veh−1 and 0.41 cm3 km−1 veh−1 are calculated. Traffic-induced turbulence has been identified to have a decisive influence on exhaust gas dispersion near the source.  相似文献   

16.
《Chemosphere》2007,66(11):1949-1958
Detailed analyses of persistent organic pollutants (POPs) such as organochlorine pesticides (OCPs), hexachlorocyclohexane (HCH) isomers (HCHs), dichlorodiphenyltrichloro ethane (DDT) and its metabolites (DDTs) and congeners of polychlorinated biphenyls (PCBs) in soil and surface water from the northeastern São Paulo, Brazil allowed the evaluation of the contamination status, distribution and possible pollution sources. The pesticides and PCBs demonstrated markedly different distributions, reflecting different agricultural, domestic and industrial usage in each region studied. The ranges of HCH, DDT, and PCBs concentrations in the soil samples were 0.05–0.92, 0.12–11.01, 0.02–0.25 ng g−1 dry wt, respectively, and in the surface water samples were 0.02–0.6, 0.02–0.58 and 0.02–0.5 ng l−1, respectively. Overall elevated levels of DDT and PCB were recorded in region 2, a site very close to melting, automotive batteries industries, and agricultural practice regions. High ratios of metabolites of DDT to DDT isomers revealed the recent use of DDT in this environment. The sources of contamination are closely related to human activities, such as domestic and industrial discharge, street runoff, agricultural pesticides and soil erosion, due to deforestation as well as atmospheric transport.  相似文献   

17.
The concentrations of total gaseous mercury (TGM) in air over the southern Baltic Sea and dissolved gaseous mercury (DGM) in the surface seawater were measured during summer and winter. The summer expedition was performed on 02–15 July 1997, and the winter expedition on 02–15 March 1998. Average TGM and DGM values obtained were 1.70 and 17.6 ng m−3 in the summer and 1.39 and 17.4 ng m−3 in the winter, respectively. Based on the TGM and DGM data, surface water saturation and air-water fluxes were calculated. The results indicate that the seawater was supersaturated with gaseous mercury during both seasons, with the highest values occurring in the summer. Flux estimates were made using the thin film gas-exchange model. The average Hg fluxes obtained for the summer and winter measurements were 38 and 20 ng m−2 d−1, respectively. The annual mercury flux from this area was estimated by a combination of the TGM and DGM data with monthly average water temperatures and wind velocities, resulting in an annual flux of 9.5 μg m−2 yr−1. This flux is of the same order of magnitude as the average wet deposition input of mercury in this area. This indicates that reemissions from the water surface need to be considered when making mass-balance estimates of mercury in the Baltic Sea as well as modelling calculations of long-range transboundary transport of mercury in northern Europe.  相似文献   

18.
The effects of natural compounds on reducing formaldehyde emission from plywood were investigated. Urea, catechin and vanillin were examined as the natural formaldehyde reducers. The microemission cell, with an internal volume of 35 ml, the maximum exposed test surface area of 177 cm2 and an air purge flow rate of 50 ml min−1, was used to measure specific emission rate (SER). In the case of no reducer treatment, formaldehyde emission from plywood was fast and SERs were 4.4 mg m−2 h−1 at 30 °C and 15 mg m−2 h−1 at 60 °C. When this plywood was treated with the natural compounds, the SERs of formaldehyde were decreased at all temperatures. In the case of urea treatment, the SERs of formaldehyde decreased to 0.30 mg m−2 h−1 at 30 °C and 0.65 mg m−2 h−1 at 60 °C. When the urea treatment was applied to the inside of kitchen cabinet (made from plywood; 270 cm wide, 60 cm deep, 250 cm high), the concentration of formaldehyde was reduced substantially from 1600 to 130 μg m−3. The reducing effect of formaldehyde continued during the observation period (6 months), with a mean concentration of 100 μg m−3. Reducers in the plywood would react with released formaldehyde. Application of natural compounds such as urea, catechin and vanillin could provide a simple and effective approach for suppressing formaldehyde emission from plywood.  相似文献   

19.
20.
The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σsp) at 525 nm, PM10, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m−1, 157.6±270.0 μg m−3, and 2.30±3.41 m2 g−1, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m−1, 119.0±112.9 μg m−3, and 1.87±1.41 m2 g−1. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM10, σsp, and α were 184.1±211.548 μg m−3, 126.3±89.6 M m−1, and 1.05±0.97 m2 g−1, respectively, and these values at Dongsheng were 146.4±142.1 μg m−3, 183.4±81.7 M m−1, and 1.98±1.52 m2 g−1, respectively. However, in winter at Dunhuang PM10, σsp, and α were 158.1±261.4 μg m−3, 303.3±165.2 M m−1, and 3.17±1.93 m2 g−1, respectively, and these values at Dongsheng were 155.7±170.1 μg m−3, 304.4±158.1 M m−1, and 2.90±1.72 m2 g−1, respectively. σsp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.  相似文献   

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