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1.
Yu K  DeLaune RD  Boeckx P 《Chemosphere》2006,65(11):2449-2455
Wetland loss along the Louisiana Gulf coast and excessive nitrate loading into the Gulf of Mexico are interrelated environmental problems. Nitrate removal by soil denitrification activity was studied in a ponded freshwater marsh receiving diverted Mississippi River water for the purpose of reversing or slowing wetland loss. Labeled 15N-nitrate was applied at 3.8 g N m−2 into four replicate study plots after removing above ground vegetation. Nitrogen gas (N2) and nitrous oxide (N2O) emissions from the plots were determined by isotope ratio mass spectrometry (IRMS). Nitrous oxide emissions were also compared with the results determined by gas chromatograph (GC). Results showed that it took 2 weeks to remove the added nitrate with N2O emission occurring over a period of 4 d. The apparent denitrification dynamics were assumed to follow the Michaelis–Menten equation. The maximum denitrification rate and Km value were determined as 12.6 mg N m −2 h−1, and 6.5 mg N l−1, respectively. Therefore the maximum capacity for nitrate removal by the marsh soil would be equivalent to 110 g N m−2 yr−1, with more than 30% of nitrogen gas evolved as N2O. For typical nitrate concentrations in Mississippi River water of about 1 mg N l−1, nitrate would be removed at a rate of 14.7 g N m−2 yr−1 with N2O emission about 1.5%. A denitrification dynamic model showed that the efficiency of nitrate removal would largely depend on the water discharge rate into the ponded wetland. Higher discharge rate will result in less retention time for the water in the marsh where nitrate is denitrified.  相似文献   

2.
Uptake rates of several PCDDs, PCDFs and PCBs were measured for semipermeable membrane devices (SPMDs) under controlled conditions in bulk water and sediment. The study was performed at 19 degrees C and 11 degrees C, and water and sediment concentrations were measured during the exposure. Linear uptake rates for specific PCDD/Fs and PCBs in 19 degrees C water varied from 34 to 111 l/m2 day and in 11 degrees C water from 8.8 to 96 l/m2 day for the whole SPMD. Uptake rates at 19 degrees C sediment ranged from 9.0 to 80 mgOC/m2 day and in 11 degrees C sediment, from 3.0 to 31, mgOC/m2 day. Partitioning of the compounds between membrane and lipid was also measured during the linear uptake phase. The membrane-lipid concentration ratios ranged from 0.02 to 1.11 depending on the compound, temperature, and bulk medium.  相似文献   

3.
Su C  Puls RW 《Chemosphere》2007,67(8):1653-1662
Recent research has shown that carbonaceous solid materials and zerovalent iron (Fe(0)) may potentially be used as media in permeable reactive barriers (PRBs) to degrade groundwater nitrate via heterotrophic denitrification in the solid carbon system, and via abiotic reduction and autotrophic denitrification in the Fe(0) system. Questions arise as whether the more expensive Fe(0) is more effective than the less expensive carbonaceous solid materials for groundwater nitrate remediation, and whether there is any synergistic effect of mixing the two different types of materials. We carried out batch tests to study the nature and rates of removal of added nitrate in the suspensions of single, binary, and ternary systems of cotton burr compost, Peerless Fe(0), and a sediment low in organic carbon. Cotton burr compost acted as both organic carbon source and supporting material for the growth of indigenous denitrifiers. Batch tests showed that cotton burr compost alone removed added nitrate at a greater rate than did Peerless Fe(0) alone on an equal mass basis with a pseudo-first-order rate constant k=0.0830+/-0.0031 h(-1) for cotton burr compost and a k=0.00223+/-0.00022 h(-1) for Peerless Fe(0); cotton burr compost also removed added nitrate at a faster rate than did cotton burr compost mixed with Peerless Fe(0) and/or the sediment. Furthermore, there was no substantial accumulation of ammonium ions in the cotton burr compost system, in contrast to the systems containing Peerless Fe(0) in which ammonium ions persisted as major products of nitrate reduction. It is concluded that cotton burr compost alone may be used as an excellent denitrification medium in a PRB for groundwater nitrate removal. Further study is needed to evaluate performance of its field applications.  相似文献   

4.
R.E. Rathbun 《Chemosphere》1997,34(12):2699-2713
The effect of reaction time on the trihalomethane and nonpurgeable total organic halide formation potentials was determined by chlorinating water samples from the Mississippi, Missouri, and Ohio Rivers. Samples were collected for three seasons at 12 locations on the Mississippi from Minneapolis, Minnesota, to New Orleans, Louisiana, and on the Missouri and Ohio 1.6 kilometers above their confluences with the Mississippi. Both types of compounds formed rapidly during the initial stages of the reaction-time period, with formation rates decreasing with time. The ratio of the nonpurgeable total organic-halide and trihalomethane concentrations decreased with time, with the nonpurgeable total organic-halide compounds forming faster during the first stages of the time period and the trihalomethane compounds forming faster during the latter stages of the time period. Variation with distance along the Mississippi River of the formation rates approximately paralleled the variation of the dissolved organic carbon concentration, indicating that the rates of formation, as well as the concentrations of the compounds formed, depended on the dissolved organic carbon concentration.  相似文献   

5.
Phyu YL  Warne MS  Lim RP 《Chemosphere》2005,58(9):1231-1239
Acute (10 day) semi-static toxicity tests in which the midge, Chironomus tepperi, were exposed to atrazine and molinate were conducted in laboratory water and in river water, in the absence and presence of sediment. The bioavailability measured as median lethal concentrations (LC50) and 95% fiducial limits (FLs) of atrazine to C. tepperi in laboratory water in the absence and presence of sediment were 16.6 (14.3-19.4) and 21.0 (18.2-24.1) mg l(-1), respectively while the corresponding values in river water were 16.7 (14.7-19.0) and 22.7 (20.3-25.4) mg l(-1), respectively. For molinate, the LC50 and FL values in laboratory water in the absence and presence of sediment were 8.8 (6.8-11.4) and 14.3 (12.4-16.4) mg l(-1), respectively and the corresponding values in river water were 9.3 (7.6-11.3) and 14.5 (12.4-16.9) mg l(-1), respectively. Atrazine has low toxicity (LC50 > 10 mg l(-1)) while molinate has moderate toxicity (1 mg l(-1) < LC50 < 10 mg l(-1)) to C. tepperi. River water did not significantly (P > 0.05) reduce the bioavailability of either chemical to C. tepperi. However, the presence of sediment did significantly (P < 0.05) reduce the bioavailability of both atrazine and molinate to C. tepperi.  相似文献   

6.
Zhang S  Zhang Q  Darisaw S  Ehie O  Wang G 《Chemosphere》2007,66(6):1057-1069
An effective analytical method for simultaneously determining 16 polycyclic aromatic hydrocarbons (PAHs), 28 polychlorinated biphenyl (PCBs), and 12 pharmaceuticals and personal care products (PPCPs) has been developed to measure their concentrations in the Mississippi river waters in New Orleans, Louisiana, USA. The method involves the simultaneous extraction of the selected PAHs, PCBs, and PPCPs, from the aqueous phase by solid phase extraction using two-layer disks consisting of C(18) and SDB-XC, and collection of suspended solid in water samples by 0.2-0.6 microm filter in a single step. Target compounds adsorbed on the extraction disks were eluted with methanol, acetone, and dichloromethane. The suspended particles retained by the filter were sonically extracted using the same solvents. GC/MS was used for quantification of PAHs and PCBs directly and of PPCPs after derivatization. The analytical method was used in a 6-month field study of the Mississippi river water for contamination by PAHs, PCBs, and PPCPs and the following concentrations (ng/l) have been obtained: clofibric acid (3.2-26.7), ibuprofen (0-34.0), acetaminophen (24.7-65.2), caffeine (0-38.0), naproxen (0-135.2), triclosan (8.8-26.3), bisphenol A (0-147.2), carbamazepine (42.9-113.7), estrone (0-4.7), 17beta-estradiol (0-4.5), total PAHs (62.9-144.7), and total PCBs (22.2-163.4).  相似文献   

7.
Organic substrates in reactive barrier systems are often heterogeneous material mixtures with relatively large contrasts in hydraulic conductivity and porosity over short distances. These short-range variations in material properties imply that preferential flow paths and diffusion between regions of higher and lower hydraulic conductivity may be important for treatment efficiency. This paper presents the results of a laboratory column experiment where denitrification is investigated using a heterogeneous reactive substrate (sawdust mixed with sewage sludge). Displacement experiments with a non-reactive solute at three different flow rates are used to estimate transport parameters using a dual porosity non-equilibrium model. Parameter estimation from breakthrough curves produced relatively consistent values for the fraction of the porosity consisting of mobile water (β) and the mass transfer coefficient (α), with average values of 0.27 and 0.42 d(-1), respectively. The column system removes >95% of the influent nitrate at low and medium flow, but only 50-75% of the influent nitrate at high flow, suggesting that denitrification kinetics and diffusive mass transfer rates are limiting the degree of treatment at lower hydraulic residence times. Reactive barrier systems containing dual porosity media must therefore consider mass transfer times in their design; this is often most easily accommodated by adjusting flowpath length.  相似文献   

8.
Virtapohja J  Alen R 《Chemosphere》1999,38(1):143-154
Laboratory-scale microcosm tests were carried out in sea water with and without sediment to investigate the importance of ultraviolet (UV) light and microbes in the temperature-dependent degradation of metal complexes of ethylenediaminetetraacetic acid (EDTA). After 17 weeks, 44% and 48% of the original EDTA (initial concentration 385 microg/L) were converted at 10 degrees C and 22 degrees C, respectively. The degradation was more influenced by UV light than by sediment microbes, although the latter were very important. At both temperatures, absorption of EDTA to the sediment phase reached a maximum in the initial stage of the experiments (<4 weeks): at 10 degrees C about 4% and at 22 degrees C about 7% of the original EDTA.  相似文献   

9.
Chemical and microbiological aspects were investigated with regard to biological denitrification of drinking water using the seaweed Gracilaria verrucosa as the carbon and energy substrate and as physical support for the microbial flora in semibatch, fixed-bed reactors. Complete removal of nitrate (100 mg/L) was readily achieved without accumulation of nitrite. Microbiological analysis indicated that the effluent of the reactor contained high numbers of bacteria (>10(6)/mL total count). Among the 44 bacterial strains isolated directly from the samples or isolated after enrichment at 37 degrees C, 25 different fatty acid profiles were found, indicating a complex microflora, including potential pathogens.  相似文献   

10.
Eggen T  Majcherczyk A 《Chemosphere》2006,62(7):1116-1125
Zero-valent iron improves the transformation of DDT [1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane] and its metabolites in aged and highly contaminated lake sediment under biotic conditions. The addition of Fe0 has a strong effect on transformation rates at 22 degrees C and 9 degrees C, the most enhanced degradation being obtained for DDT and DDOH [2,2-bis(p-chlorophenyl)ethanol]. At 22 degrees C and 10 weeks' incubation, the DDT concentration is reduced from 2.75 micromol g(-1) (974 mg kg(-1)) to 0.98 micromol g(-1) (346 mg kg(-1)) and 1.98 micromol g(-1) (702 mg kg(-1)) in samples with and without the addition of iron, respectively. After 40 weeks' incubation these concentrations have further decreased to 0.19 micromol g(-1) (66 mg kg(-1)) and 0.74 micromol g(-1) (264 mg kg(-1)).There is no significant transformation of any of the compounds at 9 degrees C without the addition of Fe0. In the presence of iron, however, DDT is reduced to 1.25 micromol g(-1) (442 mg kg(-1)) within 40 weeks' incubation. This study demonstrates the ability of adapted microorganisms to transform DDT under elevated temperatures in original, aged sediments, and also the stimulating effect of zero-valent iron, which is significant even at low temperatures.  相似文献   

11.
Water in the urban front-range corridor of Colorado has become an increasingly critical resource as the state faces both supply issues as well as anthropogenic degradation of water quality in several aquifers used for drinking water. A proposed development (up to 1100 homes over two quarter-quarter sections) at Todd Creek, Colorado, a suburb of Westminster located about 20 miles northeast of Denver, is considering use of onsite wastewater systems (OWS) to treat and remove domestic wastewater. Local health and environmental agencies have concerns for potential impacts to local water quality. Nitrogen treatment in the vadose zone and subsequent transport to ground water at a development scale is the focus of this investigation. The numerical model HYDRUS 1D was used, with input based on site-specific data and several transport parameters estimated from statistical distribution, to simulate nitrate concentrations reaching ground water. The model predictions were highly sensitive to mass-loading of nitrogen from OWS and the denitrification rate coefficient. The mass loading is relatively certain for the large number of proposed OWS. However, reasonable values for the denitrification rate coefficients vary over three orders of magnitude. Using the median value from a cumulative frequency distribution function, based on rates obtained from the literature, resulted in simulated output nitrate concentrations that were less than 1% of regulatory maximum concentrations. Reasonable rates at the lower end of the reported range, corresponding to lower 95% confidence interval estimates, result in simulated nitrate concentrations reaching groundwater above regulatory limits.  相似文献   

12.
Denitrification in the river estuaries of the northern Baltic Sea   总被引:3,自引:0,他引:3  
Estuaries have been suggested to have an important role in reducing the nitrogen load transported to the sea. We measured denitrification rates in six estuaries of the northern Baltic Sea. Four of them were river mouths in the Bothnian Bay (northern Gulf of Bothnia), and two were estuary bays, one in the Archipelago Sea (southern Gulf of Bothnia) and the other in the Gulf of Finland. Denitrification rates in the four river mouths varied between 330 and 905 micromol N m(-2) d(-1). The estuary bays at the Archipelago Sea and the Gulf of Bothnia had denitrification rates from 90 micromol N m(-2) d(-1) to 910 micromol N m(-2) d(-1) and from 230 micromol N m(-2) d(-1) to 320 micromol N m(-2) d(-1), respectively. Denitrification removed 3.6-9.0% of the total nitrogen loading in the river mouths and in the estuary bay in the Gulf of Finland, where the residence times were short. In the estuary bay with a long residence time, in the Archipelago Sea, up to 4.5% of nitrate loading and 19% of nitrogen loading were removed before entering the sea. According to our results, the sediments of the fast-flowing rivers and the estuary areas with short residence times have a limited capacity to reduce the nitrogen load to the Baltic Sea.  相似文献   

13.
Agricultural ditches primarily serve to remove and store excess water associated with irrigation and storm events. The ability of these ecosystems to mitigate potential contaminants is not well understood. Five sites along a 650-m agricultural ditch located in the Mississippi Delta Management Systems Evaluation Area (MDMSEA) were used to measure fate and effects of an esfenvalerate (insecticide) exposure. Following a 0.64-cm simulated storm event, samples were collected from water and sediments and analyzed spatially from five sites and temporally from 0.5 h to 56 d. Results of aqueous toxicity bioassays indicated that lethality progressed downstream throughout all sampling intervals, while sediment toxicity bioassays only elicited biological responses at the point of pesticide application to the ditch (0 m). Significant reductions in survival of Ceriodaphnia dubia and Pimephales promelas in water were measured at the 0-, 20-, and 80-m sites following application. Ten-day solid phase sediment testing of Chironomus tentans indicated persistent toxicity only at the point of application (0 m) and throughout 56 d (mean=14.4% survival). No lethality or significant reduction in midge growth was measured for remaining downstream sites. These measurements were used to evaluate the potential of agricultural ditches to reduce potential deleterious effects of contaminants in agricultural drainage systems that precede receiving streams.  相似文献   

14.
底泥污染物释放动力学研究   总被引:13,自引:1,他引:13  
采用模拟试验方式和新型微生物数量测定方法 ,研究了沼泽化湖泊底泥和受污染河流底泥在不同扰动状态下 ,底泥耗氧速率、氮和磷污染物释放动力学过程。结果表明 :( 1)底泥耗氧速率是同样条件下上覆水耗氧速率的 48倍 ,而在扰动状态下 ,底泥耗氧速率达到上覆水耗氧速率的 5 96— 93 6倍 ,扰动底泥显著增大其耗氧速率 ,底泥污染越严重 ,其耗氧速率越大 ,对水体产生的影响也越大。 ( 2 )扰动底泥可以显著增大底泥的氮磷释放速率 ,氮的释放受有机氮的氨化、氨氮的硝化、硝酸盐氮的反硝化以及氨氮被微生物吸收转化为有机氮等的影响 ;磷的释放过程受厌氧过程和底泥颗粒吸附的影响 ,耗氧速率高的底泥具有更大的氮磷释放潜力。 ( 3 )微生物数量在底泥污染物释放动力学中起着关键性作用 ,新型方法可以快速检测微生物总量。试验结果对于水环境的管理、受污染水体的修复 ,以及底泥的处理处置等都具有重要的指导意义  相似文献   

15.
Transport and reduction of nitrate in a typically macroporous clayey till were examined at variable flow rate and nitrate flux. The experiments were carried out using saturated, large diameter (0.5 m), undisturbed soil columns (LUC), from a forest and nearby agricultural sites. Transport of nitrate was controlled by flow along the macropores (fractures and biopores) in the columns. Nitrate reduction (denitrification) determined under active flow mainly followed first order reactions with half-lives (t(1/2)) increasing with depth (1.5-3.5 m) from 7 to 35 days at the forest site and 1-7 h at the agricultural site. Nitrate reduction was likely due to microbial degradation of accumulated organic matter coupled with successive consumption of O2 and NO3- in the macropore water followed by reductive dissolution of Fe and Mn from minerals along the macropores. Concentrations of total organic carbon measured in soil samples were near identical at the two study sites and consequently not useful as indicator for the observed differences in nitrate reduction. Instead the high reduction rates at the agricultural site were positively correlated with elevated concentration of water-soluble organic carbon and nitrate-removing bacteria relative to the forest site. After high concentrations of water-soluble organic carbon in the columns from the agricultural site were leached they lost their elevated reduction rates, which, however, was successfully re-established by infiltration of new reactive organics represented by pesticides. Simulations using a calibrated discrete fracture matrix diffusion (DFMD) model could reasonably reproduce the denitrification and resulting flux of nitrate observed during variable flow rate from the columns.  相似文献   

16.
Jäntti H  Hietanen S 《Ambio》2012,41(2):161-169
Primary production in the eutrophic Baltic Sea is limited by nitrogen availability; hence denitrification (natural transformation of nitrate to gaseous N2) in the sediments is crucial in mitigating the effects of eutrophication. This study shows that dissimilatory nitrate reduction to ammonium (DNRA) process, where nitrogen is not removed but instead recycled in the system, dominates nitrate reduction in low oxygen conditions (O2 <110 μM), which have been persistent in the central Gulf of Finland during the past decade. The nitrogen removal rates measured in this study show that nitrogen removal has decreased in the Gulf of Finland compared to rates measured in mid-1990s and the decrease is most likely caused by the increased bottom water hypoxia.  相似文献   

17.
Sediment denitrification rate and its role in removal of dissolved nitrate load in lower Ishikari river system were examined. Denitrification rate were measured using acetylene inhibition technique on the sediment samples collected during August 2009–July 2010. The denitrification rate varied from 0.001 to 1.9 μg N g−1 DM h−1 with an average value of 0.21 μg N g−1 DM h−1 in lower Ishikari river system. Denitrification rate showed positive correlation with dissolved nitrate concentration in the river basin, indicating overlying water column supplied nitrate for the sediment denitrification processes. Nutrient enrichment experiments result showed that denitrification rate increased significantly with addition of nitrate in case of samples collected from Barato Lake however no such increase was observed in the samples collected from Ishikari river main channel and its major tributaries indicating that factors other than substrate concentration such as population of denitrifier and hydrological properties of stream channel including channel depth and flow velocity may affects the denitrification rate in lower Ishikari river system. Denitrification rate showed no significant increase with the addition of labile carbon (glucose), indicating that sediment samples had sufficient organic matter to sustain denitrification activity. The result of nutrient spiraling model indicates that in- stream denitrification process removes on an average 5% d−1 of dissolve nitrate load in Ishikari river. This study was carried out to fill the gap present in the availability of riverine denitrification rate measurement and its role in nitrogen budget from Japanese rivers characterize by small river length and high flow rate.  相似文献   

18.
The mass transport model TEOTIL was used to project nitrate (NO3) fluxes from the Tovdal River basin, southernmost Norway, given four scenarios of climate change. Forests, uplands, and open water currently account for 90% of the NO3 flux. Climate scenarios for 2071-2100 suggest increased temperature by 2-4 degrees C and precipitation by 3-11%. Climate experiments and long-term monitoring were used to estimate future rates of nitrogen (N) leaching. More water will run through the terrestrial catchments during the winter but less will run in the spring. The annual NO3 flux from the Tovdal River to the adjoining Topdalsfjord is projected to remain unchanged, but with more NO3 delivered in the winter and less in the spring. Algal blooms in coastal waters can be expected to occur earlier in the year. Major sources of uncertainty are in the long-term fate of N stored in soil organic matter and the impacts of forest management.  相似文献   

19.
Soil dissipation of the herbicide clopyralid (3,6-dichloropicolinic acid) was measured in laboratory incubations and in field plots under different management regimes. In laboratory studies, soil was spiked with commercial grade liquid formulation of clopyralid (Versatill, 300 g a.i. L(-1) soluble concentrate) @ 0.8 microg a.i. g(-1) dry soil and the soil water content was maintained at 60% of water holding capacity of the soil. Treatments included incubation at 10 degrees C, 20 degrees C, 30 degrees C, day/night cycles (25/15 degrees C) and sterilized soil (20 degrees C). Furthermore, a field study was conducted at the Waikato Research Orchard near Hamilton, New Zealand starting in November 2000 to measure dissipation rates of clopyralid under differing agricultural situations. The management regimes were: permanent pasture, permanent pasture shielded from direct sunlight, bare ground, and bare ground shielded from direct sunlight. Clopyralid was sprayed in dilute solution @ 600 g a.i. ha(-1) on to field plots. Herbicide residue concentrations in soil samples taken at regular intervals after application were determined by gas chromatograph with electron capture detector. The laboratory experiments showed that dissipation rate of clopyralid was markedly faster in non-sterilized soil (20 degrees C), with a half-life (t1/2) of 7.3 d, than in sterilized soil (20 degrees C) with t1/2 of 57.8 d, demonstrating the importance of micro-organisms in the breakdown process. Higher temperatures led to more rapid dissipation of clopyralid (t1/2, 4.1 d at 30 degrees C vs 46.2 d at 10 degrees C). Dissipation was also faster in the day/night (25/15 degrees C) treatment (t1/2, 5.4 d), which could be partly due to activation of soil microbes by temperature fluctuations. In the field experiment, decomposition of clopyralid was much slower in the shaded plots under pasture (t1/2, 71.5 d) and bare ground (t1/2, 23.9 d) than in the unshaded pasture (t1/2, 5.0 d) and bare ground plots (t1/2, 12.9 d). These studies suggest that environmental factors such as temperature, soil water content, shading, and different management practices would have considerable influence on rate of clopyralid dissipation.  相似文献   

20.
Huwe J  Hakk H  Lorentzsen M 《Chemosphere》2007,67(2):259-266
Cyanogenic glycosides are common plant toxins. Toxic hydrogen cyanide originating from cyanogenic glycosides may affect soil processes and water quality. In this study, hydrolysis, degradation and sorption of dhurrin (4-hydroxymandelonitrile-beta-d-glucoside) produced by sorghum has been studied in order to assess its fate in soil. The log K(ow) of dhurrin was -1.18+/-0.08 (22 degrees C). Hydrolysis was a first-order reaction with respect to dhurrin and hydroxyl ion concentrations. Half lives ranged from 1.2h (pH 8.6; 25 degrees C) to 530d (pH 4; 25 degrees C). The activation energy of hydrolysis was 112+9kJ. At pH 5.8 and room temperature, addition of humic acids (50gl(-1)) increased the rate of hydrolysis tenfold, while addition of kaolinite or goethite (100-250gl(-1)) both decreased the rate considerably. No significant sorption to soil components could be observed. The degradation rates of dhurrin in top and subsoils of Oxisols, Ultisols, Alfisols and Mollisols were studied at 22 degrees C (25mgl(-1), soil:liquid 1:1 (w:V), pH 3.8-8.1). Half-lives were 0.25-2h for topsoils, and 5-288h in subsoils. Hydrolysis in solution explained up to 45% of the degradation in subsoils whereas the contribution in topsoils was less than 14%, indicating the importance of enzymatic degradation processes. The highest risk of dhurrin leaching will take place when the soil is a low activity acid shallow soil with low content of clay minerals, iron oxides and humic acids.  相似文献   

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