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1.

Purpose

Obtaining a better understanding of the concentrations and origins of polycyclic aromatic hydrocarbons (PAHs) in the sediments Taihu Lake, China, is of paramount importance for the environmental protection and remediation of this lake. To investigate temporal and spatial variations in PAH concentrations, composition and possible source categories, 29 sediment samples were collected from Taihu Lake during both the flooding and dry seasons of the lake.

Materials and methods

Fifteen US Environmental Protection Agency priority PAHs were detected in 58 surface sediments (29 for each season) by gas chromatograph/mass selective detection, following extraction by accelerated solvent extraction.

Results and discussion

The concentrations of the total and individual PAHs in the flooding season were higher than those in the dry season, suggesting that high levels of fishing activity may be an important contributor to PAH pollution in the flooding season. The fractions of high molecular weight PAHs in the flooding season ranged from 63?% to 71?% and were higher than those in the dry season (which ranged from 52?% to 65?%). These results indicate that vehicle exhaust may be a more important pollutant source in the flooding season than in the dry season. Diagnostic ratios, principal component analysis and hierarchical cluster analysis were used to study possible source categories in the different seasons. Consistent results were obtained for all techniques. Seasonal and spatial variations were also investigated by the coefficient of divergence method. The results of previous studies support the conclusion of source identification.

Conclusions

Vehicle emissions were the dominant contributor to PAHs in the flooding season, while PAHs in the dry season sediments may have come from multiple sources. The findings of this study may provide a theoretical basis for seasonal PAH control strategies for Taihu Lake.  相似文献   

2.

Goal, Scope and Background

Distribution of hydrophobic organic contaminants in abiotic compartments is essential for describing their transfer and fate in aquatic ecosystems. Taihu Lake is the third largest freshwater lake in China. Water quality of Taihu Lake has deteriorated greatly during the last decades and has threatened the water supply. The aim of the present study was to investigate the partitioning of polycyclic aromatic hydrocarbons (PAHs) among overlying water, suspended particulate matter (SPM), sediments, and pore water in Meiliang Bay, Taihu Lake and to provide useful information for the ecological engineering in this area.

Materials and Methods

Overlying water and surface sediment were sampled from six sites in Meiliang Bay, Taihu Lake, China. Within 72 h of sampling, sediments were centrifuged to obtain the pore water. Overlying water samples were filtered to separate dissolved and SPM samples. After extraction, samples were purified following a clean-up procedure. PAH fraction was obtained by elution with a mixture of hexane: DCM (7:3, V/V) and analyzed by GC/MS.

Results

PAHs concentrations in overlying water varied from 37.5 ng/L to 183.5 ng/L. Concentrations of PAHs in pore water were higher than those in overlying water. The total concentrations of 16 priority PAHs in sediments ranged from 2091.8 ng/g-dw to 4094.4 ng/g-dw. PAHs concentrations on SPM were decreased with suspended solid concentrations (SSC). Total PAHs concentrations on SPM varied in the range of 3369.6 ng/g-dw to 7531.1 ng/g-dw. The partition coefficients between sediment and overlying water (log K oc) for PAHs with log K ow<5 were positively correlated with their octanol-water partition coefficients (log K ow) (n=39, r=0.79, p<0.0001). Partition coefficients between sediment and pore water (log K oc′) for all PAHs were also significantly correlated with their log K ow values (n=48, r=0.82, p<0.0001).

Discussion

In general, PAHs derived from combustion sources tend to bind strongly to soot particles in natural sediment. Consequentially, K oc values observed in the natural environment could be orders of magnitude higher than those predicted by linear correlation relationships under laboratory conditions. In the present study, the ratio of log K oc values to log K ow values falls consistently above 1, indicating that the sediment soot carbon in the bay was more attractive for PAHs than n-octanol. The log K oc′ was also higher than that predicted under laboratory conditions, suggesting that the measured pore water PAH concentrations were lower than those predicted. That is to say, not all the sediment PAHs can be available to partition rapidly into sediment pore waters. A variation in soot content is a possible reason. Furthermore, concentrations of PAHs on SPM were higher than those in sediments. The compositions of PAHs on SPM and in sediments were similar, indicating the importance of re-suspension process of sediments in the partitioning process of the shallow lake.

Conclusions

The results indicated the equilibrium partitioning model could be used to predict PAHs distribution in various phases of a shallow lake in the stagnation period, but re-suspension processes should be considered to modify the relationship between log K ocs and log K ows.

Recommendations and Perspectives

Concentration, particle size and composition of resuspended particles could affect the relationship between log K ocs and log K ows. Further work should be done under field conditions, especially where a steady thermodynamic equilibrium state could be assumed.
  相似文献   

3.

Purpose

Polycyclic aromatic hydrocarbons (PAHs) are unintentional products that are classified as persistent toxic substances. The goal of the present study was to generate data on the presence of 15 priority PAHs that are found in surface sediment and core sediment in the region of the Turvo/Grande watershed, São Paulo State, Brazil, which is an area of expanding sugarcane cultivation, and to correlate these data with the sources of these PAHs and the guiding values for sediment quality analysis.

Materials and methods

Surface sediments and sediment cores were sampled during the rainy and dry seasons in February and July 2010. The extraction of PAHs from sediments was performed using a Soxhlet extractor, and then the extract was cleaned according to the methods of the US EPA 3630C (US EPA 1996) using a silica gel column. Quantification was performed using high performance liquid chromatography with fluorescence detection.

Results and discussion

The concentrations of all 15 PAHs decreased as the depth of the sediment core increased. Overall, the concentrations decreased along the sediment core; however, the RTURARG (region predominantly used for planting sugarcane and livestock) during the rainy season and the CAPRP sampling site (located at part of the Preto River dam) during the dry season showed increased concentrations in the first few sediment fractions, and then the concentrations decreased. Higher concentrations were observed in urban locations, and the concentration of naphthalene was higher than the probable effect level (PEL) determined by the Canadian environmental agency. The obtained diagnostic ratios indicate that the sediment from areas with an abundance of sugarcane was a pyrolytic source of PAHs, which indicates a contribution from burning straw to the PAH concentrations in those areas.

Conclusions

For all sampling sites and all PAHs, we found a decreasing trend in PAH concentrations with increasing sediment core depth, and the locations, such as CAPRP, that experienced a higher level of human activity had the highest total concentrations of PAHs. These locations were the only areas in which the PAH naphthalene was found in higher concentrations than the PEL. The diagnostic ratios reveal that regions with sugarcane plantations had predominantly pyrolytic sources of PAHs, indicating the contribution of PAHs from sugarcane straw burning.
  相似文献   

4.

Purpose

Determining the dynamics of silicon in lakes, one of the essential nutrients for diatoms, is valuable for understanding aquatic environmental problems. The dissolved silicon (DSi) and biogenic silicon (BSi) budgets in Lake Kasumigaura, a shallow eutrophic lake in Japan, during the last three decades were assessed based on the analysis of dated sediment cores and a water quality database.

Materials and methods

Sediment cores (100?cm long) were taken at the center of Lake Kasumigaura in 2005, 2007, and 2009 and at two other sites in 2007. BSi contents of the dated sediments were determined by wet alkaline digestion. The net sedimentation rates of BSi were defined as the difference between the DSi load from inflowing rivers and the DSi and BSi loads from the outflow of the lake, calculated using DSi concentrations and diatom abundances in the lake from 1980 to 2007 and DSi concentrations of the inflowing rivers during 1994, 2007, and 2009. The gross sedimentation rates of BSi were estimated by multiplying BSi concentrations in lake water by the diatom sinking rate reported by previous studies.

Results and discussion

Budgetary calculations based on the database showed that 60?C70?% of DSi inputs from the inflowing rivers during the 27?years could ultimately be accumulated as diatom frustules in bottom sediments in the lake. The sediment analysis revealed that the amount of BSi accumulated in the lake from 1980 to 2007 was 2.0?C2.6?×?1011?g, similar to the amount based on the database of 1.3?C2.4?×?1011?g. Although the gross sedimentation rates of BSi likely increased, the net sedimentation rates of BSi decreased significantly from 6?C10?×?109?g?year?1 in the 1980s to 2?C6?×?109?g?year?1 in the 2000s, suggesting a fast recycling of BSi in recent years caused by an increase in sediment resuspension and regeneration.

Conclusions

The sediment core information and the water quality database can be used for calculating the long-term silicon budgets in Lake Kasumigaura. An increase in the DSi release rates was identified, which is consistent with recent sediment resuspension. Comparing the sediment core information with the database suggests the long-term dissolution of sediment BSi; however, analysis of the BSi content in sediment cores representing a much longer time period is needed to confirm this.  相似文献   

5.

Purpose

Understanding the fate and behavior of polycyclic aromatic hydrocarbon (PAH) sources in aquatic systems is important for the efficiency of control policies. In this work, a new approach??organic carbon-normalized sediment?Cpore water partition coefficients of PAH source contributions (logK??Osource)??was developed to study the sediment?Cpore water partition of PAH source contributions. The focus of this study was the Yellow River, which is the second largest river in China and one of the largest rivers in the world.

Materials and methods

Sixteen priority US Environmental Protection Agency PAHs were analyzed in 14 surface sediments and 11 pore water samples. Principal component analysis?Cmultiple linear regression (PCA-MLR) and Unmix models were employed to estimate the source contributions of PAHs in sediments and pore water samples. Finally, logK??Osource values were calculated according to the modeled source contributions of PAHs.

Results and discussion

??PAHs (sum of the 16 PAH concentrations) in 14 sediment samples and 11 pore water samples from the Yellow River were 1,415?±?726?ng?g?1 dry weight (dw) and 123?±?57.4???g?l?1, respectively. The source apportionment results indicate the following: (1) for sediment samples, the contributions to ??PAHs from vehicular emissions, coal combustion, and petrogenic sources were 41.07?C61.05, 38.83?C45.56, and 11.18?C14.92?%, respectively, and (2) for pore water samples, vehicular emissions were the most significant contributor (45.51?C69.39?%), followed by petrogenic sources (29.80?C34.22?%) and coal combustion (7.35?C21.59?%). Coal combustion had the highest logK??Osource values (4.15?C4.26) among the three categories, followed by vehicular emissions (3.51?C3.57) and petrogenic sources (3.30?C3.43).

Conclusions

The possible categories of PAH sources identified by hierarchical cluster analysis, PCA-MLR, and Unmix models were consistent, indicating that vehicular emissions, coal combustion, and petrogenic sources were three important categories. The logK??Osource values indicate that contributions from coal combustion had a higher partition for the sediment phase compared with the other two source categories.  相似文献   

6.

Purpose

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous and persistent contaminants in aquatic bed sediments. A better understanding of their in-bed fate and transport is therefore key in minimising the risk to the environment over time through various remediation and monitoring strategies. Since ecological effects and risks are related to contaminant concentrations, this study developed CoReTranS, a predictive model that simulates one-dimensional organic contaminant reaction and transport in bed sediments.

Materials and methods

CoReTranS was benchmarked against analytical solutions of simplified reactive transport models and validated using a published study of marsh sediments contaminated with petroleum-derived hydrocarbons from Wild Harbour, West Falmouth, MA, USA.

Results and discussion

The CoReTranS model effectively predicted the vertical distribution of PAHs in the Wild Harbour sediments as confirmed by the modelling results from the published study. The CoReTranS model was also used to interpret results from a published study of PAH-contaminated fjord sediments from Kitimat Arm in British Columbia, Canada. Specific insights into the post-depositional fate and transport of selected PAHs in the Kitimat fjord sediments were obtained by comparing the measured concentration-depth profiles with the numerical results from the CoReTranS model. Key parameters such as effective diffusivity of contaminants and burial velocities of sediment particles were shown to possibly account for the predicted concentrations-depth profiles in the Kitimat fjord sediments.

Conclusions

As demonstrated, CoReTranS can simulate reactive transport models in order to predict PAH concentration profiles in porewater under site-specific conditions. The information derived from the use of the CoReTranS model highlighted practical application of such information by engineers to site-specific risk assessment and remediation.  相似文献   

7.

Purpose

This study addresses the feasibility of a flotation technique, using a lab-scale flotation cell, to simultaneously remove both metals and polyaromatic hydrocarbons (PAHs) from fine sediment fractions (<250 μm) that are potentially contaminated with copper (Cu).

Materials and methods

A multiple flotation process with three consecutive flotation stages was performed on three sediments (13S, 14B, and 24A) with different particle size distributions, Cu and PAH concentrations, and organic matter contents.

Results and discussion

Flotations performed under selected conditions allowed for significant removal of both Cu (61–70 %) and PAHs (75–83 %) with acceptable froth recoveries of approximately 23–29 %. Removal rates for arsenic, lead, and zinc were 48–61, 40–48, and 32–36 %, respectively. Flotation selectivity of Cu was greatly influenced by the contents of fine particles and organic matter of the sediments. The maximum flotation selectivity was obtained for the 53–125-μm size fraction. The high flotation selectivity of Cu (2.5–3.2) and PAHs (3.0–3.6) demonstrated the feasibility of flotation to treat soils or sediments containing both organic and inorganic pollutants.

Conclusions

Overall, the flotation results showed a high selectivity for both Cu and PAHs and demonstrated the feasibility of flotation to treat media contaminated with organic and inorganic contaminants.  相似文献   

8.

Purpose

A multi-compartment monitoring study was performed to characterize the effect of environmental variables, such as temperature and water flow as well as sediment characteristics, on the distribution and transport of persistent organic pollutants (POPs) in a dynamic river system during 1 year in an industrial region in central Europe.

Materials and methods

Waterborne polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) were assessed over a period of 1 year at five sampling sites in the Morava River in the Czech Republic. Contaminants were measured monthly in riverbed sediments, freshly deposited sediments, water samples and passive samplers.

Results and discussion

Sediments are the main carrier of POPs in the river. Distinguishable patterns of PAHs, OCPs and PCBs in sediment indicate that their origin is from distinct sources and different transport pathways. The PAHs were identified as the dominant contaminant group of compounds with a mean concentration in sediment of 5,900 μg kg?1. Such concentrations are up to 10 times higher than in the Danube River, into which Morava drains. In contrast, mean concentrations of PCBs, hexachlorocyclohexanes (HCHs), dichlorodiphenyltrichloroethane and its breakdown products (DDTs) and hexachlorobenzene (HCB) of 6.0, 0.4, 4.2 and 6.0 μg kg1, respectively, are similar to those in the Danube. With some exceptions, no significant difference in composition of surficial riverbed sediments and those collected using sediment traps was observed. Despite the presence of potential local pollutant sources, the differences in contaminant concentrations between sites in the region were in most cases not significant. Variations in POP concentrations in sediments are mainly induced by high flow events, whereas seasonal variability was not observed.

Conclusions

The changes in contaminant concentrations in Morava River sediments are induced by episodic high flow events that cause erosion of contaminant-containing particles and their deposition at suitable downstream sites.  相似文献   

9.

Purpose

The management of sediments from stormwater infiltration basins is nowadays a key issue for local authorities to ensure long-term performance. Speciation of pollutants is particularly required in view of reuse of these materials. If fractionation of trace metals in sediments is relatively well described, polycyclic aromatic hydrocarbons (PAHs) speciation was only studied using particle size distribution. Therefore, this study aims at the characterization of the PAHs-bearing fractions in sediments.

Materials and methods

Three sediments with various physicochemical properties were sampled in the west and north of France to characterize the distribution of PAHs among organic and inorganic components. Respective organic and inorganic matrixes were obtained by alkaline extraction and methyl isobutyl ketone (MIBK) fractionation procedure. The nature of the solid fractions was assessed through microanalyses: infrared spectroscopy (Fourier transform infrared spectroscopy), X-ray diffraction (XRD), and scanning electron microscopy with X-ray spectroscopy. Bulk sediments and extracted fractions were analyzed for organic matter parameters: elemental analysis (C, N, and H), total organic matter, total organic carbon, hydrocarbons (C10–C40), and PAHs.

Results and discussion

The characterization of bulk sediments highlighted that they were mainly composed of single particles, originating from the geological background, and aggregates (10 to 300 μm) composed of minerals and large organic matter content. The C/N ratio and PAH ratios were shown to be helpful for the determination of the natural or anthropogenic origin of organic matter or to evaluate additional contribution of industrial activities. The fractionation results underlined the role of the aggregates on the distribution of PAHs. Humin fraction and bound-humic acids were mainly composed of aggregates (10 to 150 μm) and accounted for 60 to 70 % of sample mass. The PAHs are mainly sequestrated in these fractions. Only up to 1 % of PAHs are adsorbed on the mineral fraction.

Conclusions

Both alkaline extraction and MIBK procedure demonstrated that PAH residues were readily sequestrated in humin and bound-humic acids fractions and that fulvic acids, humic acids, and mineral fractions contained poor concentrations of PAHs. Microanalyses underlined the high level of aggregation of particles in sediments and their mixed inorganic and organic nature. In case of stormwater sediments, the location of PAHs in highly organic aggregates is consistent with their sources, being both oil products and debris from vehicles and road.  相似文献   

10.

Purpose

During the late 1950s and early 1960s, industrial waste material highly enriched with various contaminants (e.g., heavy metals, polycyclic aromatic hydrocarbons (PAHs)) was dumped in the inner Bay of Mecklenburg, western Baltic Sea. Between 2002 and 2004, a research program was initiated using chemical analysis in combination with bioanalytical techniques to assess the extent and variability in contamination at this dump site (DS). The data were compared to a reference area (RS) with similar environmental conditions, which is representative of the western Baltic Sea.

Materials and methods

Twelve PAHs were investigated to assess their ecological hazard, as they were identified as major pollutants in the dumped material. In addition to analyzing the actual PAH contamination status in the sediments, PAHs measured in the soft tissue of Arctica islandica were also used as an indicator of contaminant bioaccumulation. A biotest battery was applied to determine the toxic effects of contaminants in the sediment.

Results and discussion

Significantly elevated PAH concentrations (sum of 12 PAHs) of ~3,000 ng g?1 dw and higher bioaccumulation factors (BAFs) were determined in the soft body tissue of A. islandica collected at DS (t test, p?=?0.025). The results also showed that the sediment PAH contamination was significantly higher at DS (1,952–5,466 ng g?1 dw) than at RS (1,384–2,315 ng g?1 dw). The results revealed a major heterogeneity in the PAH concentration at DS due to an attempt to cover the toxic material with clean clay. This resulted in a more heterogeneous distribution of the dump material rather than covering it up completely. However, not all relevant contaminants were included in this study, not only because it is too costly to determine them all but also because unidentified contaminants present at concentrations below the limit of detection cannot be measured. Bioassays were used to fill this gap in the hazard assessment in a cost-effective way by investigating the possible effects of sediment contamination on benthic organisms. The results showed a high variability and magnitude of growth and luminescence inhibition. Bacterial contact tests with marine organisms showed a high toxicity response (>80 % inhibition) from DS sediments. In contrast, the luminescent bacteria test (Vibrio fischeri) showed equivalent effects of sediments from both DS and RS.

Conclusions

The spatial distribution of toxicity in DS, the bioaccumulation in mussels and the analytical evidence of PAH pollution clearly show that the dumped material still represents a potential risk even after 60 years.  相似文献   

11.

Purpose

Sediment contamination in US waterways is an expensive and complicated issue, and as acceptance of nontraditional sediment remediation strategies broadens, novel and efficient methods to assess and monitor the bioavailability of hydrophobic organic contaminants (HOCs) in contaminated sediments will play an important role.

Materials and methods

In this project, solid phase microextraction (SPME) fibers inside perforated steel tubes were used as in situ passive samplers to measure polycyclic aromatic hydrocarbon (PAH) concentrations in sediment before and after treatment with activated carbon (AC). Two modes of waterjet amendment injection were used to apply the AC. In the first treatment, a single 2-min injection was shot into the center of a test vessel, and in the second treatment, multiple 7-s injections in a grid were placed in sediment.

Results and discussion

In the single injection, no treatment was observed 5 cm away from the injection, while at 2.5 cm, >90 % decrease of PAH pore water concentration was observed, indicating a similar bioavailability decrease. In the multiple injection experiment, >90 % PAH pore water level reductions were observed throughout the test vessel. Highly contaminated and less contaminated sediments were mixed with 0–5 % AC by weight to develop AC treatment curves. Over 99 % reduction in PAH pore water concentrations and bioavailability was observed in the less contaminated sediment at 3 % AC, while 99 % reduction was never reached even at 5 % AC addition in the highly contaminated sediment. Different treatment curves were observed for the different contaminated sediments. In situ equilibration times were 120, 215, and 250 h for phenanthrene, pyrene, and benzo(a)anthracene, respectively.

Conclusions

The results show that in situ SPME is a viable method to observe AC treatment and evaluate reductions in pore water concentrations and bioavailability.  相似文献   

12.
Specific stability of organic matter in a stormwater infiltration basin   总被引:1,自引:0,他引:1  

Purpose

In stormwater infiltration basins, sediments accumulate at the soil surface and cause a gradual filling up of soil pores. These sediments are composed of a mixture of natural and anthropogenic (as oil products) organic matters (OMs). The degradation kinetics of these sediment OMs and their biological stability has been neglected. This study aimed to characterize sediments OMs to assess their evolution and their capacity to degrade.

Materials and methods

To characterize OMs from the sediment layer, we measured at several places in the infiltration basin, total OM and carbon (C) contents, C distribution and biochemical fractions of the OM in the different size fractions, the sediment’s C mineralization potential, soil microbial biomass, and organic pollutants (polycyclic aromatic hydrocarbons (PAHs)) in the sediment layer.

Results and discussion

OM contents were high and varied from 66 to 193 g?kg?1 from the inlet to the outlet of basin. Depending on rainfall intensity and volume, organic particles were deposited at varying distances in the basin by decantation; this was confirmed by analysis of sediment C distribution in the different size fractions. Despite high amounts of OM, organic C had a low biodegradability. Mineralization potentials were low compared to natural soil (i.e., from 0.3 to 1.1 g CO2–C kg?1 total organic carbon). Biochemical fractionation of the organic fractions indicated that they were mainly composed of a soluble fraction, which contributed to reducing OM biodegradability. The activity of the sediment microbial biomass was low. PAH contents seemed to be partly responsible for the high biostability of OMs.

Conclusions

There was limited capacity for biodegradation of sediment OMs probably due to inhibitory effects of soluble PAHs and consequently low microbial activity.  相似文献   

13.

Purpose

Phosphorus (P) is a limiting nutrient for most US Midwestern aquatic systems and, therefore, increases of P, through point or non-point sources (NPS) of pollution such as agriculture, causes eutrophication. Identifying specific NPS contributions (e.g., upland vs. stream channels) for sediments and P is difficult due to the distributed nature of the pollution. Therefore, studies which link the spatial and temporal aspects of sediment and P transport in these systems can help better characterize the extent of NPS pollution.

Materials and methods

Our study used fingerprinting techniques to determine sources of sediments in an agricultural watershed (the North Fork of the Pheasant Branch watershed; 12.4 km2 area) in Wisconsin, USA, during the spring, summer, and fall seasons of 2009. The primary sources considered were uplands (cultivated fields), stream bank, and streambed. The model used fallout radionuclides, 137Cs, and 210Pbxs, along with total P to determine primary sediment sources. A shorter-lived fallout radioisotope, 7Be, was used to determine the sediment age and percent new sediments in streambed and suspended sediment samples (via the 7Be/210Pbxs ratio).

Results and discussion

Upland areas were the primary source of suspended sediments in the stream channels followed by stream banks. The sediment age and percent new sediment for the streambed and suspended sediments showed that the channel contained and transported newer (or more recently tagged with 7Be) sediments in the spring season (9–131 days sediment age), while relatively old sediments (165–318 days) were moving through the channel system during the fall season.

Conclusions

Upland areas are the major contributors to in-stream suspended sediments in this watershed. Sediment resuspension in stream channels could play an important role during the later part of the year. Best management practices should be targeted in the upland areas to reduce the export of sediments and sediment-bound P from agricultural watersheds.  相似文献   

14.

Purpose

Factors such as organic matter can significantly influence the distribution of mercury (Hg) in aquatic environments. Recent studies in Arctic and sub-Arctic lakes in Canada have investigated whether scavenging of Hg by phytoplankton significantly affects distributions of Hg in sediments. This study examined the relationships between Hg and organic components in two contrasting lakes (Lakes Qinghai and Chenghai) in low and middle latitudes of China.

Materials and methods

Sediment cores from the less-polluted, oligotrophic Lake Qinghai (QH) and from the polluted, eutrophic Lake Chenghai (CH) were collected by a gravity corer. The cores were sectioned and transported on ice to the laboratory where they were stored at ?20 °C. Subsamples were dried in a vacuum freeze dryer and grounded with a mortar and pestle prior to analyses. Total concentrations of Hg were quantified using cold vapor atomic absorption spectrometry. Total organic carbon (TOC) was quantified using an elemental analyzer after removal of carbonate. The Rock-Eval 6 pyrolysis technique (Vinci Technologies, Rueil-Malmaison, France) was used to deconvolute TOC in sediments into S1, S2, and RC components; S2 was further separated into S2a and S2b.

Results and discussion

Different relationships between Hg and TOC were found in the two lakes, which suggest that different types of organic compounds might play completely different roles in the distribution of Hg in lakes. S1 (the soluble organic matter (SOM)) was found to significantly control distributions of Hg in sediments of both lakes, while S2 and S2a were not. Combining the synchronous fluctuations of Hg and the oxygen index in the QH sediment core and in recent sections of CH suggested that allochthonous SOM derived from the terrestrial environment had an important influence on the distribution of Hg in both lakes and a large portion of Hg that originated from the lake catchment.

Conclusions

This study provides further evidence that organic matter is one of the most important factors that influences distributions of Hg in lake sediments and that SOM was the primary form of carbon associated with sedimentation of Hg. The results also suggest that Hg in lake sediments might not accurately represent its pollution history as it could also be influenced by land use, such as agriculture or other human activities in the catchment.  相似文献   

15.

Purpose

Sediments adversely impact the quality of surface waters and are a significant source of contaminants, such as nutrients and pesticides, in agricultural watersheds. The development of effective beneficial management practices (BMPs) to minimize these impacts requires a sound understanding of the sources of sediments. The objectives of this study were: (1) to determine the sources of sediment in an agricultural watershed in the Canadian prairies using sediment source fingerprinting and; (2) to assess the results of the sediment fingerprinting study within the context of the scale of observation and the hydro-geomorphic connectivity of the watershed.

Materials and methods

Geochemical and radionuclide fingerprints were used to discriminate between the three potential sediment sources identified: topsoil, streambanks, and shale bedrock. Suspended and bed sediment samples were collected over the course of 3 years at six locations along the main stem of the creek, ranging from 3rd- (48 ha) to 7th-order (7441 ha) drainage basins. Four sediment fingerprint properties were selected that met statistical- and process-based selection criteria and the Stable Isotope Analysis in R model was used to estimate the proportion of sediment derived from each source at each sampling location in the watershed.

Results and discussion

The suspended sediments in the upper reaches were dominated by topsoil sources (64%–85%), whereas the suspended sediments moving through the lower reaches and being exported from the watershed had a higher proportion of sediment coming from streambank (32%–51%) and shale bedrock (29%–40%) sources. The switch in the sources of sediment between the headwaters and the watershed outlet are due to: (1) changes in sediment storage and connectivity; (2) a transition in the dominant erosion processes from topsoil to streambank erosion; and (3) the incision of the stream through the shale bedrock as it crosses the Manitoba Escarpment.

Conclusions

The results of this sediment fingerprinting study demonstrated that there was a switch in sediment sources between the headwaters and the outlet of the watershed. This research highlights the importance of the sampling location, in relation to the scale and geomorphic connectivity of the watershed, on the interpretation of results derived from the sediment fingerprinting technique, particularly in terms of developing suitable watershed BMPs to protect surface waters.  相似文献   

16.

Purpose

The Todos os Santos Bay is the largest bay in Brazil and receives drainage from various watersheds. For more than 450 years, it was the main destination for the domestic and hospital sewage from the city of Salvador, Bahia. With the growing concern regarding the presence of pharmaceutical and personal care products (PPCPs) in the environment, an investigation was undertaken to determine the presence and levels of some commonly used drugs (i.e., atenolol, caffeine, carbamazepine, diazepam, diclofenac, erythromycin, ibuprofen) and personal care products (i.e., galaxolide, tonalide), using sediments as an indicator of their presence in the water column.

Material and methods

Surficial sediment samples from 17 stations located in the intertidal zone of the Todos os Santos Bay and infralittoral zone along the north coast of Salvador were tested for the presence of some PPCPs using LC-MS/MS (for drugs) and GC-MS/MS (for fragrances).

Results and discussion

The PPCPs examined were present in all sediment samples at levels of parts per billion of dry sediment. The highest concentrations were found for the fragrances galaxolide (52.5 ng g?1) and tonalide (27.9 ng g?1), followed by caffeine (23.4 ng g?1) and pharmaceuticals ibuprofen (14.3 ng g?1), atenolol (9.84 ng g?1), carbamazepine (4.81 ng g?1), erythromycin (2.29 ng g?1), diclofenac (1.06 ng g?1), and diazepam (0.71 ng g?1).

Conclusions

Pharmaceuticals were found to be ubiquitous in the sediments of the study areas. The texture of the sediment was an important factor in PPCPs fixation and deposition. The concentrations of all PPCPs had statistically significant positive correlations with the percentage of clay in the sediments.  相似文献   

17.

Purpose

Microbial sulfate reduction is an alkalinity-producing process and potentially supports the neutralization of acidic mine pit lakes. In many acidic lakes the process does not occur. Sulfate-reducing bacteria are known to be pH sensitive. There are, however, several reports of sulfate reduction occurring in the sediment of acidic lakes. To find out why sulfate reduction occurs in some acidic lakes but not in others, we conducted a field experiment.

Materials and methods

Surface sediment from lake ML111 (pH?2.6, no sulfate reduction), in the Koyne-Plessa lignite mining district of Lusatia in Germany, was incubated in the less-acidic lake ML117 (pH?3.4, sulfate reduction) and vice versa. After 19?weeks of incubation, the sediments were sampled and analyzed for microbial sulfate reduction rates, bacterial numbers, and geochemical composition.

Results and discussion

Incubation of ML117 sediment in ML111 resulted in a partial inhibition of sulfate reduction while incubation of ML111 sediment in ML117 did not initiate sulfate reduction. We observed a linear relationship between sediment pH and sulfate reduction, while there was no relation with sedimentary iron content. Sulfate reduction was not only affected by the water quality but also by the experimental treatment. Homogenization of the sediment prior to incubation stimulated microbial sulfate and iron reduction. Due to the low pH, incubation in ML111 resulted in the dissolution of reduced inorganic sulfur.

Conclusions

We conclude that the water pH is the major regulator of sulfate reduction in the surface sediment of acidic lakes. The rate of sulfate reduction in the sediment of acidic lakes depends on a fragile equilibrium between proton flux between water and sediment, and buffering reactions in the sediment.  相似文献   

18.

Purpose

Suspended particulate sediment (SPS) concentration has a great impact on the sediment to water partitioning coefficients (K p) of hydrophobic organic compounds (HOCs), which is called the particle concentration effect (PCE). However, the mechanisms regarding the PCE are not yet well understood, and there is little direct experimental evidence for these mechanisms. The aim of this study was to investigate the PCE of polycyclic aromatic hydrocarbon (PAH) sorption on sediment by analyzing the freely dissolved concentrations of PAHs.

Materials and methods

Sediments were collected from the Yellow River and the Haihe River in China. Pyrene was selected as a model PAH to investigate the sorption of PAH on sediments. In addition to the total dissolved concentration (C TW) of pyrene, the freely dissolved concentration (C FW) measured by polyethylene devices was used to investigate the PCE of pyrene in the presence and absence of phenanthrene and chrysene.

Results and discussion

For both the Haihe River and Yellow River sediments, in the presence and absence of other PAHs, the K p value of pyrene with C FW as the equilibrium concentration in the water phase was approximately two times higher than that with C TW as the equilibrium concentration. With either C TW or C FW as the equilibrium concentration in the water phase, the K p value of pyrene decreased with increasing SPS concentration as a power function. In addition, the K p value with C TW as the equilibrium concentration decreased faster than that with C FW. This inferred that, apart from a third phase including dissolved organic carbon (DOC) and colloids, particle–particle, or particle–DOC interactions were important for the PCE. The contribution of the third phase to the PCE for the Haihe River sediment (72.5?±?26.4 %) was greater than the contribution for the Yellow River sediment (48.4?±?16.2 %), which had a larger particle size and lower total organic carbon and black carbon contents.

Conclusions

The PCE of PAH sorption onto sediments was attributed to both the third phase and to particle–particle or particle–DOC interactions. The contribution of the third phase to the PCE depended on both the TOC content and the particle size of sediment. As high SPS and DOC concentrations exist in many rivers, their effects on the sorption of HOCs should be considered when conducting bioavailability and ecological risk assessment.  相似文献   

19.

Purpose

The geochemical compositions of sediments from three sectors in Trincomalee Bay (Koddiyar Bay, Thambalagam Bay and the Inner Harbour) in Sri Lanka were examined to determine fluvial and marine contributions and the effects of sorting and heavy mineral concentration. The present environmental status of the bay was also assessed.

Materials and methods

Forty-nine sediment samples were collected from Trincomalee Bay and analysed by X-ray fluorescence, yielding data for the major elements and 17 trace elements. Mean grain size and sorting were also measured. Data were compared with the compositions of sediments from the lower Mahaweli River, which supplies most of the clastic detritus to Trincomalee Bay.

Results and discussion

Sediments in the three sectors differ significantly in chemical composition, according to position relative to the Mahaweli River delta source, depositional environment, heavy mineral concentration and marine influences. According to accepted sediment quality guidelines, some As contamination may have occurred in the Inner Harbour and Thambalagam Bay and Cr contamination in all three sectors.

Conclusions

Proximal Koddiyar Bay sediments compare closely with Mahaweli River bedload. Although the clastic component in the more distal Thambalagam Bay and the Inner Harbour is also derived from the Mahaweli River, compositions are modified significantly by marine contributions. High concentrations of elements including Ti, Zr, Ce, Nb and Y in NW Koddiyar Bay are consistent with heavy mineral concentration by winnowing in high-energy zones. Some decoupling of Fe–Ti- and Zr-bearing heavy mineral assemblages may occur within the bay. Al-normalized metal enrichment factors and contour maps show that apparent contamination by As and Cr is spurious and is caused by locally high background levels from Mahaweli River detritus. This illustrates the importance of establishing local background levels of elements during environmental studies.  相似文献   

20.

Purpose

A comprehensive study was conducted to investigate the presence of polycyclic aromatic hydrocarbons (PAHs) in Dongjiang River Basin (DRB) soils and to evaluate their sources and ecological and health risk. In addition, factors affecting the distribution and fate of PAHs in the soils such as emission density, soil organic matter, degradation, etc. were studied.

Materials and methods

Surface soil (0–20 cm) samples from 30 sampling sites in the rural areas of DRB were collected and analyzed for 17 polycyclic aromatic hydrocarbons (16 EPA priority PAHs and perylene). Positive matrix factorization model was used to investigate the source apportionment of these PAHs, and an incremental lifetime cancer risk (ILCR) was used to estimate the integrated lifetime risks of exposure to soil-borne PAHs through direct ingestion, dermal contact, and inhalation collectively.

Results and discussion

The total PAH concentrations in the rural soils in DRB range from 23.5 to 231 μg/kg with a mean concentration of 116 μg/kg. The predominant PAHs in the rural soils were naphthalene, fluoranthene, phenanthrene, and benzo(b)fluoranthene. Cluster analysis was performed to classify the soil PAHs into three clusters, which could be indicative of the soil PAHs with different origins and different properties. Source apportionment results showed that coal, biomass, oil, commercial creosotes, and vehicle contributed 24 %, 24 %, 17 %, 17 %, and 18 % of the total soil PAH burden, respectively. The ILCR results indicated that exposure to these soil-borne PAHs through direct ingestion, dermal contact, and inhalation collectively produces some risk.

Conclusions

PAHs in the soils of the DRB will produce long-term influences on rivers and oceans via soil erosion and river transport. Therefore, PAHs in rural soils of DRB have potential impacts on the water supply and human health risk.  相似文献   

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