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1.
In this study rates of oxygen, ammonium (NH4 +), nitrate (NO3 −), nitrite (NO2 −), and nitrous oxide (N2O) fluxes, nitrogen (N) fixation, nitrification, and denitrification were compared between two intertidal sites for which there is an abundant global literature, muddy and sandy sediments, and two sites representing the rocky intertidal zone where biogeochemical processes have scarcely been investigated. In almost all sites oxygen production rates greatly exceeded oxygen consumption rates. During daylight, NH4 + and NO3 − uptake rates together with ammonification could supply the different N requirements of the primary producer communities at all four sites; N assimilation by benthic or epilithic primary producers was the major process of dissolved inorganic nitrogen (DIN) removal; N fixation, nitrification, and denitrification were minor processes in the overall light DIN cycle. At night, distinct DIN cycling processes took place in the four environments, denitrification rates ranged from 9 ± 2 to 360 ± 30 μmol N2 m−2 h−1, accounting for 10–48% of the water column NO3 − uptake; nitrification rates varied from 0 to 1712 ± 666 μmol NH4 + m−2 h−1. A conceptual model of N cycle dynamics showed major differences between intertidal sediment and rocky sites in terms of the mean rates of DIN net fluxes and the processes involved, with rocky biofilm showing generally higher fluxes. Of particular significance, the intertidal rocky biofilms released 10 times the amount of N2O produced in intertidal sediments (up to 17 ± 6 μmol N2O m−2 h−1), representing the highest N2O release rates ever recorded for marine systems. The biogeochemical contributions of intertidal rocky substrata to estuarine and coastal processes warrant future detailed investigation.  相似文献   

2.
《Applied Geochemistry》2003,18(5):765-779
Stable isotope systematics of C, N and S were studied in soils of 5 European forest ecosystems. The sites were located along a North–South transect from Sweden to Italy (mean annual temperatures from +1.0 to +8.5 °C, atmospheric deposition from 2 to 19 kg N ha−1 a−1, and from 6 to 42 kg S ha−1 a−1). In Picea stands, the behavior of C, N and S isotopes was similar in 3 aspects: (1) assimilation favored the lighter isotopes 12C, 14N and 32S; (2) mineralization in the soil profile left in situ residues enriched in the heavier isotopes 13C, 15N and 34S; and (3) NO3–N as well as SO4–S in soil solution was isotopically lighter compared to the same species in the atmospheric input. In this study, emphasis was placed on S isotope profiles which so far have been investigated to a much lesser extent than those of C and N. Sulfate in monthly samples of atmospheric input had systematically higher δ34S ratios than total soil S at the 0–5 cm depth, on average by 4.0‰. Sulfate in the atmospheric input had higher δ34S ratios than in deep (>50 cm) lysimeter water, on average by 3.2‰. Organic S constituted more than 50% of total soil S throughout most of the profiles (0–20 cm below surface). There was a tendency to isotopically heavier organic S and lighter inorganic SO4–S, with ester SO4–S heavier than C-bonded S at 3 of the 5 sites. With an increasing depth (0 to 20 cm below surface), δ13C, δ15N and δ34S ratios of bulk soil increased on average by 0.9, 4.2 and 1.6‰, respectively, reflecting an increasing degree of mineralization of organic matter. The isotope effects of C, N and S mineralization were robust enough to exist at a variety of climate conditions and pollution levels. In the case of S, the difference between isotope composition of the upper organic-rich soil horizon (lower δ34S) and the deeper sesquioxide-rich soil horizons (higher δ34S) can be used to determine the source of SO4 in streams draining forests. This application of δ34S as a tracer of S origin was developed in the Jezeřı́ catchment, Czech Republic, a highly polluted site suffering from spruce die-back. In 1996–1997, the magnitude and δ34S of atmospheric input (20 kg S ha−1 a−1, 5.8‰) and stream discharge (56 kg S ha−1 a−1, 3.5‰) was monitored. Export of S from the catchment was 3 times higher than contemporary atmospheric input. More than 50% of S in the discharge was represented by release of previously stored pollutant S from the soil. Stable isotope systematics of Jezeřı́ soil S (mean of 2.5‰ in the O+A horizon, 4.8‰ in the B horizon, and 5.8‰ in the bedrock) suggests that most of the soil-derived S in discharge must come from the isotopically light organic S present in the upper soil horizon, and that mineralized organically-cycled S is mainly flushed out during the spring snowmelt. The fact that a considerable proportion of incoming S is organically cycled should be considered when predicting the time-scale of acidification reversal in spruce die-back affected areas.  相似文献   

3.
Sediment-water exchanges of ammonium (NH4 +), nitrate + nitrite (NOx ?), filterable reactive phosphorus (FRP, primarily ortho-phosphate), and oxygen (O2) under aphotic (heterotrophic) conditions were determined at 2–5 stations in the Neuse River Estuary, from 1987 to 1989. Shallow (1 m), sandy stations were sampled along the salinity gradient. Fluxes from deep (>2 m) sites were compared to the shallow sites in two salinity zones. Grain size became finer and organic content increased with depth in the oligohaline zone but not in the mesohaline zone. Net release of NH4 + and FRP occurred at all sites. Fluxes varied from slight uptake to releases of 200–500 μmol m?2 h?1 (NH4 +) and 150–900 μmol m?2 h?1 (FRP). Net NOx ? exchange was near zero, but were ±100 μmol m?2 h?1 over the year. Release of NH4 + and FRP from the shallow sandy stations decreased with distance down the estuary, but O2 uptake did not change. The deeper oligohaline site had twofold higher rates of NH4 + and FRP release and O2 uptake than the shallow site, but no differences occurred between depths in the mesohaline zone. Temperature and organic content were important controls for all fluxes, but water column NOx ? concentration was also important in regulating NOx ? exchanges. Ratios of oxygen consumption to NH4 + release were near the predicted ratio (Redfield model) at oligohaline sites but increased down estuary at mesohaline sites. This may be due to greater nitrification rates promoted by autotrophy in the sediments.  相似文献   

4.
《Applied Geochemistry》2002,17(7):903-921
Farm waste stores such as cattle slurry lagoons are widespread in the UK and many overly important aquifers. Stores can be serious risks to water quality because they are important sources of N species, organic C and pathogenic microbes. At two sites on the Chalk aquifer of southern England, inclined boreholes were drilled and cored to obtain aquifer material from directly beneath unlined slurry stores. Vertical boreholes were also drilled adjacent to the slurry stores to determine any lateral movement of contaminants. Interstitial porewaters were analysed for major and minor ions and S isotopes. At the second site, unsaturated zone gases were sampled from the inclined hole. Infiltration of slurry into the unsaturated zone caused significantly elevated concentrations of metals such as Cu and Ni at both sites. Sulphate reduction was occurring at Site 1, as evidenced by SO4 concentrations decreasing from 150 to 50 mg/l and enhanced ratios of δ34S–SO4 and δ18O–SO4. Ammonium-N also leaches along with dissolved organic C which were found 17 m below ground surface at concentrations up to 400 and 260 mg/l, respectively. Contaminant concentrations were similar in the porewaters from both the inclined and vertical boreholes. At Site 2, higher contaminant concentrations were found in the inclined borehole compared with the vertical borehole. Organic C concentrations were considerably lower than at Site 1, ranging from 10 to 70 mg/l. Ammonium–N concentrations reached a maximum concentration of 25 mg/l, however NO3-N concentrations were up to 500 mg/l and SO4 concentrations were generally higher than Site 1. Data for N2/Ar and δ15N–N2 from the gas samplers show a peak of 102 and 2.2‰, respectively, at 14 m below ground level indicating denitrification was taking place. Evidence from δ34S–SO4 and δ18O–SO4 suggest that some SO4 reduction was taking place simultaneously. From CH4 and NH3 detected at depth it is suggested that slurry contamination, emanating from early use of the store, has passed through the top 18 m of the unsaturated zone at Site 2. The presence of high concentrations of NO3 and lower concentrations of organic C suggests that this lagoon has formed a relatively impermeable seal at its base within the first few years of its lifetime. The anoxic conditions at both sites may have mobilised U from N–P–K fertilisers. Both sites are continuing to impact on the porewater chemistry and pose a risk of groundwater contamination.  相似文献   

5.
Benthic nitrogen (N) cycling was investigated at six stations along a transect traversing the Peruvian oxygen minimum zone (OMZ) at 11°S. An extensive dataset including porewater concentration profiles and in situ benthic fluxes of nitrate (NO3−), nitrite (NO2−) and ammonium (NH4+) was used to constrain a 1-D reaction-transport model designed to simulate and interpret the measured data at each station. Simulated rates of nitrification, denitrification, anammox and dissimilatory nitrate reduction to ammonium (DNRA) by filamentous large sulfur bacteria (e.g. Beggiatoa and Thioploca) were highly variable throughout the OMZ yet clear trends were discernible. On the shelf and upper slope (80-260 m water depth) where extensive areas of bacterial mats were present, DNRA dominated total N turnover (?2.9 mmol N m−2 d−1) and accounted for ?65% of NO3− + NO2− uptake by the sediments from the bottom water. Nonetheless, these sediments did not represent a major sink for dissolved inorganic nitrogen (DIN = NO3− + NO2− + NH4+) since DNRA reduces NO3− and, potentially NO2−, to NH4+. Consequently, the shelf and upper slope sediments were recycling sites for DIN due to relatively low rates of denitrification and high rates of ammonium release from DNRA and ammonification of organic matter. This finding contrasts with the current opinion that sediments underlying OMZs are a strong sink for DIN. Only at greater water depths (300-1000 m) did the sediments become a net sink for DIN. Here, denitrification was the major process (?2 mmol N m−2 d−1) and removed 55-73% of NO3− and NO2− taken up by the sediments, with DNRA and anammox accounting for the remaining fraction. Anammox was of minor importance on the shelf and upper slope yet contributed up to 62% to total N2 production at the 1000 m station. The results indicate that the partitioning of oxidized N (NO3−, NO2−) into DNRA or denitrification is a key factor determining the role of marine sediments as DIN sinks or recycling sites. Consequently, high measured benthic uptake rates of oxidized N within OMZs do not necessarily indicate a loss of fixed N from the marine environment.  相似文献   

6.
A comparative experiment was conducted in two cross sections with sandy and sandy loam sediment textures along an agricultural drainage stream in eastern China to address the effects of sediment texture on in-stream nitrogen uptake efficiency. Using dimerous chambers for in situ incubations, NO3-N and NH4-N uptake metrics (i.e., areal uptake rate and uptake velocity) and associated hydrochemical variables in the enclosed sediment–water column system were measured for 8 days and two nights across April–July in 2011 and March–June in 2012. For the investigated sites, in-stream uptake accounted for 2–45 and 9–36 % of the initial NH4-N and NO3-N within the enclosed water column, respectively. Although similar daytime, diel and day-to-day (daytime) variation patterns of NO3-N or NH4-N uptake metrics were observed for the two sites, the sandy loam sediments had average net NO3-N and NH4-N uptake efficiency ~50 % higher and ~40 % lower than for the sandy sediments, respectively. As NO3-N was the dominant nitrogen form in the studied water columns (typical of agricultural drainage rivers), the sandy loam sediment site had an average of about 47 % higher net uptake efficiency for dissolved inorganic nitrogen (i.e., NO3-N + NH4-N). This study demonstrates that sediment texture has a considerable effect on spatial variation of nitrogen uptake along the river system. Changing sediment texture due to anthropogenic modifications on catchment land use and stream channels has the potential to change stream nitrogen cycling as well as altering nitrogen inputs and forms to downstream aquatic ecosystems.  相似文献   

7.
The effects of molecular diffusivity of H2SO4 and NH3 vapours on nucleated particles of SO42− and NO3− species are reported. Condensation sink and source rate of H2SO4 and NH3 vapours, growth rates and ratios of real to apparent nucleation rates are calculated for SO4– and NO3− aerosols using fractional contributions of them in total aerosol size-distribution during the measurement period at Pune, reported in Chate and Pranesha (2004). The percentage of nucleated SO42− and NO3− aerosols of mid-point diameter 13 nm are 2% and 3% respectively of the total particles (13 nm ≤ D p ≤ 750 nm) for both H2SO4 and NH3 diffusion. In the diameter range 75 nm ≤ D p ≤ 133 nm, it is 48% and 45% of SO42− and NO3− aerosols, respectively for NH3 diffusion and 43% and 36% of SO42− and NO3− for H2SO4 diffusion. Increase in percentage of nucleated particles of these species corresponding to mid-point diameter 133 nm around 0900 h IST is significantly higher than that of mid-point diameter 13 nm and it is due to photo-chemical nucleation, coagulation and coalescence among nucleated clusters. The ratios of real to apparent formation rates for SO42− and NO3− aerosols are 12% and 11% respectively, corresponding to mid-point diameter 13 nm, 17% and 13%, for midpoint diameter 133 nm and 12% and 9.5%, for mid-point diameter 750 nm. The results indicate that nucleation involving H2SO4 and acidic NH3 diffusion on SO42− and NO3− particles is the most relevant mechanism in this region.  相似文献   

8.
Temporal variations in the concentration and N isotopic ratios of inorganic N (NH4– and NO3–N) as affected by the soil temperature regime together with the input of bird excreta were analyzed in a sedentary soil under a dense colony (1.6 nests/m2) of breeding Black-tailed Gulls (Laruscrassirostris: a ground-nesting seabird). Surface soil samples were taken monthly from mid-March to late July 2005 from Kabushima Island, Hachinohe, northeastern Japan. The spatial concentration of inorganic N in the soils varied considerably on all sampling dates. There may be a statistically significant trend, showing increased NH4–N content from settlement up to early June when the input of fecal N attains its maximum, and then decreases towards the end of breeding activity (early August). Abundant NO3–N was observed in all soils, particularly in the later stage of breeding (up to 3800 mg-N/kg dry soil), refuting earlier claims that nitrification is unimportant in the soils. δ15N values of NH4 in the soils showed unusually high values up to +51‰, reflecting N isotope fractionation due to volatilization of NH3 during the mineralization. Mean δ15N values of the monthly collected totals of NH4 and NO3 were not significantly different at the 5% level based on ANOVA and significant differences were observed only among the three means of NO3–N collected in mid-March (settlement of colony: δ15N = −0.2 ± 3.5‰) and late July (later stages of breeding: δ15N = +22.1 ± 7.0‰, +23.3 ± 7.8‰) at the 1% and 5% levels by t-test, respectively. Such an observation of significantly increased δ15N values for NO3–N in soils from the fledgling stage indicates the integration of denitrification coupled with nitrification under a limited supply of fecal N.  相似文献   

9.
Eutrophication of lakes and reservoirs has become a worldwide environmental problem, and nitrogen (N) has been recognized as one of the key factors responsible for eutrophication. Nitrogen adsorbed on sediments may be released via chemical and biological processes under changing environmental conditions. Spatial distributions of concentrations of ammonia nitrogen (NH4 +–N), nitrate nitrogen (NO3 ?–N) and total nitrogen (TN) were investigated in sediments and overlying water of Dongting Lake, the second largest freshwater lake in China. The concentration of TN in the sediments exhibited strong spatial variation with relatively high values in the eastern part and relatively low values in the southern part of the lake. The TN concentration in the water of different regions of Dongting Lake was affected by the internal load of sediment N. The vertical distribution of TN in sediment cores showed a decreasing trend with an increase in depth. Concentrations of NH4 +–N in the sediment cores decreased with the depth increase until 6–8 cm and then increased slowly. However, concentrations of NO3 ?–N in the sediment cores showed an opposite trend from those of NH4 +–N. A kinetic release experiment of NH4 +–N showed that the maximum release rate occurred in the first 5 min and the amount of NH4 +–N release reached 77.93–86.34 % of the total amount in 0–10 min. The release of NH4 +–N in the surface sediments of Dongting Lake fits a first-order kinetics function.  相似文献   

10.
Subterranean estuaries are highly dynamic in processing dissolved inorganic nitrogen (DIN). Here we investigate DIN turnover in surface sediments (0–20 cm depth) at the higher, medium and lower intertidal of a seepage face, i.e., the outer “mouth” of the subterranean estuary, during four consecutive seasons in Sanggou Bay, China. Throughout the studied period, ammonium (NH4+) and nitrite (NO2?) concentrations in the sampled porewaters did not vary significantly with depth or season. In contrast, peaks in porewater nitrate (NO3?) concentration and decreases in δ15N-NO3? and δ18O-NO3? were observed in the 15–20 cm depth (bottom) sediment, particularly during summer and autumn. Coupled with NO3? production, the sediment total nitrogen was also markedly peaking in the bottom layer of the studied seepage face. Together with abundant heterotrophic microbes in the sediment, this NO3? accumulation was linked to a reaction chain including organic matter decomposition, ammonification and nitrification. During winter, porewater enrichment in total nitrogen occurred closer to the surface of the seepage face but triggered also active NO3? production. This pattern reinforced the importance of pelagic organic matter supply on NO3? production. In the shallower depths of the seepage face (<12 cm), active net NO3? removal occurred except in winter. The isotopic fractionation (δ15N-NO3? and δ18O-NO3?) and metagenomic results revealed denitrification as the main pathway for NO3? reduction. Biological assimilation from benthic primary producers may also consume a fraction of NO3? at the sediment water interface. Both NO3? production and removal significantly varied in magnitude with season (?13.6 to 6.2 nmol cm?3 h?1). Substrate supply was the key driver for nitrate cycling, as evidenced by the high NO3? production rate in spring by comparison to autumn. The highest NO3? turnover rates were found in summer, suggesting the combined influence of advection rates and sediment microbiota composition. In spite of active removal (peak NO3? removal capability: 61%), a significant amount of NO3? was still transported from the seepage face into the bay waters. The magnitude of NO3? fluxes ranged from 312 to 476 kg N d?1, accounting for approximately 15% of the total exogenous NO3? loading into the bay. NO3? isotopic fingerprint revealed chemical fertilizer as the main source of terrestrial NO3? in SGD, highlighting the importance of land use to coastal system nitrogen budgets.  相似文献   

11.
High concentrations of ammonium nitrogen released from tannery sludge during storage in open air may cause nitrogen pollution to soil and groundwater. To study the transformation mechanism of NH4+-N by nitrifying functional bacteria in tannery sludge contaminated soils, a series of contaminated soil culture experiments were conducted in this study. The contents of ammonium nitrogen (as NH4+-N), nitrite nitrogen (as NO2?-N) and nitrate nitrogen (as NO3?-N) were analyzed during the culture period under different conditions of pollution load, soil particle and redox environment. Sigmodial equation was used to interpret the change of NO3?-N with time in contaminated soils. The abundance variations of nitrifying functional genes (amoA and nxrA) were also detected using the real-time quantitative fluorescence PCR method. The results show that the nitrification of NH4+-N was aggravated in the contaminated silt soil and fine sand under the condition of lower pollution load, finer particle size and more oxidizing environment. The sigmodial equation well fitted the dynamic accumulation curve of the NO3?-N content in the tannery sludge contaminated soils. The Cr(III) content increased with increasing pollution load, which inhibited the reproduction and activity of nitrifying bacteria in the soils, especially in coarse-grained soil. The accumulation of NO2?-N contents became more obvious with the increase of pollution load in the fine sand, and only 41.5% of the NH4+-N was transformed to NO3?-N. The redox environment was the main factor affecting nitrification process in the soil. Compared to the aerobic soil environment, the transformation of NH4+-N was significantly inhibited under anaerobic incubation condition, and the NO3?-N contents decreased by 37.2%, 61.9% and 91.9% under low, medium and high pollution loads, respectively. Nitrification was stronger in the silt soil since its copy number of amoA and nxrA genes was two times larger than that of fine sand. Moreover, the copy numbers of amoA and nxrA genes in the silt soil under the aerobic environment were 2.7 times and 2.2 times larger than those in the anaerobic environment. The abundance changes of the amoA and nxrA functional genes have a positive correlation with the nitrification intensity in the tannery sludge-contaminated soil.  相似文献   

12.
The aim of this study was to evaluate the relative performance of three nitrification inhibitors (NIs) viz. calcium carbide (CaC2), and plant derivatives of Pongamia glabra Vent. (karanj) and Melia azedarach (dharek) in regulating N transformations, inhibiting nitrification and improving N recovery in soil–plant systems. In the first experiment under laboratory incubation, soil was amended with N fertilizer diammonium phosphate [(NH4)2HPO4] at a rate of 200 mg N kg?1, N + CaC2, N + karanjin, and N + M. azedarach and incubated at 22 °C for 56 days period. Changes in total mineral N (TMN), NH4 +–N and NO3 ?–N were examined during the study. A second experiment was conducted in a glasshouse using pots to evaluate the response of wheat to these amendments. Results indicated that more than 92 % of the NH4 + initially present had disappeared from the mineral N pool by the end of incubation. Application of NIs i.e., CaC2, karanjin, and M. azedarach resulted in a significant reduction in the extent of NH4 + disappearance by 49, 32, and 13 %, respectively. Accumulation of NO3 ?–N was much higher in N amended soil 57 % compared to 11 % in N + CaC2, 13 % in N + karanjin, and 18 % in N + M. azedarach. Application of NIs significantly increased growth, yield, and N uptake of wheat. The apparent N recovery in N-treated plants was 20 % that was significantly increased to 38, 34, and 37 % with N + CaC2, N + karanjin, and N + M. azedarach, respectively. Among the three NIs tested, CaC2 and karanjin proved highly effective in inhibiting nitrification and retaining NH4 +–N in the mineral pool for a longer period.  相似文献   

13.
The regulatory effect of salinity on nitrogen dynamics in estuarine sediments was investigated in the Randers Fjord estuary, Denmark, using sediment slurries and intact sediment cores and applying 15N-isotope techniques. Sediment was sampled at three representative stations varying in salinity, and all experiments were run at 0‰, 10‰, 20‰, and 30‰. The sediment NH4 + adsorption capacity decreased markedly at all stations when salinity was increased from 0‰ to 10‰; further increase showed little effect. In situ nitrification and denitrification also decreased with increasing salinities, with the most pronounced reduction of approximately 50% being observed when the salinity was raised from 0‰ to 10‰. The salinity-induced reduction in NH4 + adsorption capacity and stimulation of NH4 + efflux has previously been argued to cause a reduction in nitrification activity since the nitrifying bacteria become limited by NH4 + availability at higher salinities. However, using a potential nitrification assay where NH4 + was added in excess, it was demonstrated that potential nitrification activity also decreased with increasing salinity, indicating that the inhibitory salinity effect may also be a physiological effect on the microorganisms. This hypothesis was supported by the finding that denitrification based on NO3 − from the overlying water (Dw), which is independent of the nitrification process, and hence NH4 + availability, also decreased with increasing salinity. We conclude that changes in salinity have a significant effect on nitrogen dynamics in estuarine sediments, which must be considered when nitrogen transformations are measured and evaluated.  相似文献   

14.
This paper aims to reveal the reciprocal influence of Kürtün Dam and wastewaters from the settlements on the water quality in the stream Har?it, NE Turkey. Several key water-quality indicators were measured: water temperature (T), pH, dissolved oxygen (DO), electrical conductivity, water hardness, chemical oxygen demand (COD), ammonium nitrogen (NH4 +–N), nitrite nitrogen (NO2 ?–N), nitrate nitrogen (NO3 ?–N), total Kjeldahl nitrogen (TKN), total nitrogen (TN), orthophosphate phosphorus (PO4 3?–P), and methylene blue active substances (MBAS). The monitoring and sampling studies were conducted every 15 days from March 2009 to February 2010 at two stations selected in the upstream and downstream of the Kürtün Dam. It was concluded that the Kürtün Dam Lake had a high-quality water in terms of T, pH, DO, COD, NH4 +–N, NO2 ?–N and NO3 ?–N values, but slightly polluted water with respect to TKN, PO4 3?–P, and MBAS according to the Turkish Water Pollution Control Regulation. The dam improved the stream water quality by increasing the DO concentration, and decreasing the NO2 ?–N and PO4 3?–P concentrations thanks to its hydraulic residence time despite the wastewater discharge by the nearby settlements. However, the wastewater discharge deteriorated the stream water quality increasing the COD, NH4 +–N, NO3 ––N, and TN concentrations.  相似文献   

15.
Atmospheric dust is considered to be the major cause of poor air quality due to its contribution to high particulate levels, but their interaction with the acidic gases helps in controlling the level of SO2 and NO2 through ambient neutralization reactions. In the present study, the interaction of acidic gases such as SO2 and NO2 with alkaline dust was investigated during October, 2013–July, 2014 at a site named as Babarpur located at the Trans-Yamuna region of Delhi. The concentration of SO2 ranged from 10 to 170 μg/m3 with an average of 36 μg/m3 while that of NO2 ranged from 15 to 54 μg/m3 with an average of 26?±?8 μg/m3. The results were observed to be well within the National Ambient Air Quality Standard (NAAQS) limits prescribed by the Central Pollution Control Board (CPCB). The average concentrations of SO2 during day and night time were recorded as 31?±?18 and 43?±?53 μg/m3 respectively while the mean concentrations of NO2 during day and night time were recorded as 26?±?7 and 27?±?12 μg/m3 respectively. A positive correlation between SO42? and NO3? was also observed indicating their secondary aerosol formation. In aerosol phase, average concentrations of SO42? during day and night time were 3.9?±?0.3 and 6.5?±?2.3 μg/m3 respectively while that of NO3? were 9.5?±?1.5 and 7.3?±?0.5 μg/m3 respectively. Molar ratios of Ca2+/SO42?, NH4+/SO42?, and NH4+/NO3? were observed as 8, 5, and 1.7 during daytime and 1.5, 0.4, and 0.8 during nighttime respectively. Such molar ratios confirmed high concentrations of sulphate (SO4)2? and low concentrations of nitrate (NO3?) during night time, thereby indicating different pathway of aerosol formation during day and night time. Surface morphology and elemental composition of aerosol samples showed various oval, globular, and platy shapes where the diameter varied from few nm to ~5 μm depending on their precursors. There were certain shapes like grossularite, irregular aggregate, grape-like, triangular, and flattened which indicate the crustal origin of aerosols and their possible role in SO2 and NO2 adsorption.  相似文献   

16.
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17.
《Applied Geochemistry》2000,15(9):1383-1397
Water pollution arising from base metal sulphide mines is problematic in many countries, yet the hydrogeology of the subsurface contaminant sources is rarely well-characterized. Drainage water pumped from an active F–Pb mine in northern England has unusual chemistry (alkaline with up to 40 mg.l−1 Zn) which profoundly impacts the ecology of the receiving watercourse. Detailed in-mine surveys of the quantity and quality of all ground water inflows to the mine were made. These revealed major, temporally persistent heterogeneities in ground water quality, with three broad types of water identified as being associated with distinct hydrostratigraphic units. Type I waters (associated with the Firestone Sill aquifer) are cool (<10°C), Ca–HCO3–SO4 waters, moderately mineralized (specific electrical conductance (SEC)≤410 μS.cm−1) with <4 mg.l−1 Zn. Type II waters (associated with the Great Limestone aquifer) are warmer (≈15°C), of Ca–SO4 facies, highly mineralized (SEC≤1500 μS.cm−1) with ≤40 mg.l−1 Zn. Type III waters (in the deepest workings) are tepid (>18°C), of Ca–HCO3–SO4 facies, intermediately mineralized (SEC≤900 μS.cm−1) with ≤13 mg.l−1 Zn, and with significant Fe (≤12 mg.l−1) and Pb (≤8 mg/l). Monotonic increases in temperature and Cl− concentration with depth contrast with peaks in total mineralization, SO4 and Zn at medium depth (in Type II waters). Sulphate, Pb and Zn are apparently sourced via oxidation of galena and sphalerite, which would release each metal in stoichiometric equality with SO4. However, molal SO4 concentrations typically exceed those of Pb and Zn by 2–3 orders of magnitude, which mineral equilibria suggest is due to precipitation of carbonate “sinks” for these metals. Contaminant loading budgets demonstrate that, although Type II waters amount to only 25% of the total ground water inflow to the mine, they account for almost 60% of the total Zn loading. This observation has important management implications for both the operational and post-abandonment phases of the mine life cycle.  相似文献   

18.
Hydrochemistry and isotope geochemistry of the upper Danube River   总被引：7，自引：0，他引：7  
The upper Danube River and 19 of its major tributaries were monitored for 1046 km downriver and seasonally for Ca, Mg, Sr, Na, K, HCO3, CO2, Cl, PO4, SiO2, NO3, NO2, NH4, SO4, δ13CDIC, δ18OH2O, δDH2O, δ34SSO4, δ18OSO4, and 87Sr/86Sr. Hydrological considerations and δ18O/δD data show that the water balance in the river, particularly after its confluence with the Inn, is controlled by the southern tributaries draining the Mesozoic carbonate complexes of the Alps. As a result, chemical balance at Bratislava is mostly a conservative product of its tributaries. The concentrations of Ca, Mg, and Sr in the Danube are 6 to 9 times higher than in “pristine” rivers. Although all these cations are derived from dissolution of Mesozoic carbonates, the ultimate cause is likely the enhanced generation of soil CO2 due to agricultural and forestry practices. Dissolution of Triassic sulfates is an additional factor for Ca enrichment in the headwater section of the river. Dissolved sulfate, with a comparable enrichment factor to that of alkaline earths, appears to be derived mostly from atmospheric deposition, a proposition based on consideration of its sulfur and oxygen isotopic compositions. Na, K, and Cl are enriched by a factor of 2.5 to 4 times, mostly as a result of industrial and municipal pollution sources.In contrast to the above components, which behave mostly conservatively during the downriver flow of the Danube, biogenic elements such as nutrients and Si are influenced by in-river processes. The photosynthesis/respiration balance that impacts the carbon cycle and the oxygen balance has been discussed elsewhere (Pawellek and Veizer, 1994). NO3, NO2, and NH4 are enriched by a factor of 10 to 16 times from point and diffuse sources along the watercourses, generating at times downflow nitrification plumes from NH4 to NO3. PO4 varies seasonally, chiefly as a result of biologic demand during the warm periods. For SiO2, the biological uptake (mostly for secretion of diatom frustules), combined with the deficiency of this compound that results from the predominantly carbonate lithology of the catchment, results in concentrations that are below those of pristine rivers. Overall, the present-day “salted” characteristics of the river are chiefly a consequence of the long habitation history of the upper Danube watershed.  相似文献   

19.
Benthic macroinvertebrate biomass and ammonium excretion rates were measured at four stations in the Gulf of Mexico near the Mississippi River mouth. Calculated areal excretion rates were then compared to sediment-water nitrogen fluxes measured in benthic bottom lander chambers at similar stations to estimate the potential importance of macroinvertebrate excretion to sediment nitrogen mineralization. Excretion rates for individual crustaceans (amphipods and decapods) was 2–21 nmoles NH4 + (mg dry weight)?1 h?1. The mean excretion rates for the polychaetes, Paraprionaspio pinnata [6–12 nmoles NH4 + (mg dry weight)?1h?1] and Magelona sp. [27–53 nmoles NH4 + (mg dry weight)?1h?1], were comparable or higher than previous measurements for similar size benthic or pelagic invertebrates incubated at the same temperature (22±1°C). Although the relatively high rates of excretion by these selective feeders may have been partially caused by experimental handling effects (e.g., removal from sediment substrates), they probably reflected the availability of nitrogen-rich food supplies in the Mississippi River plume. When the measured weight-specific rates were extrapolated to total areal biomass, areal macroinvertebrate excretion estimates ranged from 7 μmole NH4 + m?2h?1 at a 40-m deep station near the river mouth to 18 μmole NH4 + m?2h?1 at a shallower (28-m deep) station further from the river mouth. The net flux of ammonium and nitrate from the sediments to the water measured in bottom lander chambers in the same region were 15–53 μmole NH4 + m?2h?1 and ?25–21 μmole NO3 ? m?2h?1. These results suggest that excretion of NH4 + by macroinvertebrates could be a potentially important component of benthic nitrogen regeneration in the Mississippi River plume-Gulf shelf region.  相似文献   

20.
Sulfide Inhibition of Nitrate Removal in Coastal Sediments   总被引：1，自引：0，他引：1  
Microbial nitrate (NO3−) removal via denitrification (DNF) at high sulfide (H2S) concentrations was compared in sediment from a coastal freshwater pond in a developed area that receives salt-water influx during storm events, and a saline pond proximal to an undeveloped estuary. Sediments were incubated with added SO42− (1,000 μg per gram dry weight basis (gdw)) to determine whether acid volatile sulfides (AVS) were formed. DNF in the sediments was measured with NO3–N (300 μg gdw−1) alone, and with NO3–N and H2S (1,000 μg S2− gdw−1). SO42− addition to the freshwater sediments resulted in AVS formation (970 ± 307 μg S gdw−1) similar to the wetland with no added SO42− (986 ± 156 μg S gdw−1). DNF rates measured with no added H2S were greater in the freshwater than the wetland site (10.6 ± 0.6 vs. 6.4 ± 0.1 μg N2O–N gdw−1 h−1, respectively). High H2S concentrations retained NH4–N in the undeveloped wetland and retained NO3–N in the developed freshwater site, suggesting that potential salt-water influx may reduce the ability of the freshwater sediments to remove NO3–N.  相似文献   

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