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1.
The knowledge of the environmental fate of polycyclic aromatic hydrocarbons (PAHs) is restricted to few climatic regions of the world almost excluding the Taiga. Our objectives were to (i) separate anthropogenic from background contributions to PAH concentrations and (ii) determine temporal trends in PAH concentrations during the last century including the change in distribution of PAHs in interior and exterior portions of aggregates in soils of the Moscow region. Along a southeast-bound transect from Moscow (windward in winter) and at a background location northeast of Moscow (leeward in winter), seven topsoil samples were collected in 1910-1954 and 35 in 1998-2003. We fractionated the soils in interior and exterior portions of aggregates > 10 mm and remaining soil without aggregates. The sum of 21 PAHs (sigma21PAHs) concentrations in recent bulk soil ranged from 59 to 1350 ng g(-1). The concentrations of all PAHs were lower outside than in Moscow. The range of the concentrations of the sigma21PAHs in archived soil samples (159-1280 ng g(-1)) was similar as in recent soils. In most recent and archived samples, naphthalene and phenanthrene, were most abundant. The concentrations of low-molecular-weight PAHs decreased during the last century at most sites; those of high-molecular-weight compounds increased. The sigma21PAHs concentrations were accumulated in the exterior of aggregates (109%) and depleted in the interior (95%) relative to the concentration in bulk soil (defined as 100%), which was similar to that in the soil without aggregates (99%). The differences between aggregate interior and exterior did not change during the last century. The dominance of naphthalene and phenanthrene is typical of remote regions. The urban influence on PAH concentrations in the last century was small.  相似文献   
2.
There may be important biological sources of polycyclic aromatic hydrocarbons (PAHs) to the global environment, particularly of naphthalene, phenanthrene, and perylene, that originate in the tropics. We (i) studied the distribution of PAHs among different compartments of a typical Cerrado to locate their sources and (ii) quantified the PAH storage of this ecosystem. The sum of 20 PAH (sigma20PAHs) concentrations ranged from 25 to 666 microg kg(-1) in plant tissue, 7.4 to 32 microg kg(-1) in litterfall, 206 to 287 microg kg(-1) in organic soil, and 10 to 79 microg kg(-1) in mineral soil. Among the living biomass compartments, the bark had the highest mean PAH concentrations and coarse roots the lowest, indicating that PAHs in the plants originated mainly from aboveground sources. Naphthalene and phenanthrene were the most abundant individual PAHs, together contributing 33 to 96% to the sigma20PAHs concentrations. The total storage of the X20PAHs in Cerrado was 7.5 mg m(-2) to a 0.15-m soil depth and 49 mg m(-2) to a 2-m soil depth. If extrapolated to the entire Brazilian Cerrado region, roughly estimated storages of naphthalene and phenanthrene correspond to 7300 and 400 yr of the published annual emissions in the United Kingdom, respectively. The storage of benzo[a]pyrene, a typical marker for fossil fuel combustion, in the Cerrado only corresponds to 0.19 yr of UK emissions. These results indicate that the Brazilian savanna comprises a huge reservoir of naphthalene and phenanthrene originating most likely from the aboveground parts of the vegetation or associated organisms. Thus, the Cerrado might be a globally important source of these PAHs.  相似文献   
3.
To distinguish between pyrogenic and biological sources of PAHs in a tropical rain forest near Manaus, Brazil, we determined the concentrations of 21 PAHs in leaves, bark, twigs, and stem wood of forest trees, dead wood, mineral topsoil, litter layer, air, and Nasutitermes termite nest compartments. Naphthalene (NAPH) was the most abundant PAH with concentrations of 35 ng m(-3) in air (>85% of the sum of 21PAHs concentration), up to 1000 microg kg(-1) in plants (>90%), 477 microg kg(-1) in litter (>90%), 32 microg kg(-1) in topsoil (>90%), and 160 microg kg(-1) (>55%) in termite nests. In plants, the concentrations of PAHs in general decreased in the order leaves > bark > twigs > stem wood. The concentrations of most low-molecular weight PAHs in leaves and bark were near equilibrium with air, but those of NAPH were up to 50 times higher. Thus, the atmosphere seemed to be the major source of all PAHs in plants except for NAPH. Additionally, phenanthrene (PHEN) had elevated concentrations in bark and twigs of Vismia cayennensis trees (12-60 microg kg(-1)), which might have produced PHEN. In the mineral soil, perylene (PERY) was more abundant than in the litter layer, probably because of in situ biological production. Nasutitermes nests had the highest concentrations of most PAHs in exterior compartments (on average 8 and 15 microg kg(-1) compared to <3 microg kg(-1) in interior parts) and high PERY concentrations in all compartments (12-86 microg kg(-1)), indicating an in situ production of PERY in the nests. Our results demonstrate that the deposition of pyrolytic PAHs from the atmosphere controls the concentrations of most PAHs. However, the occurrence of NAPH, PHEN, and PERY in plants, termite nests, and soils at elevated concentrations supports the assumption of their biological origin.  相似文献   
4.
We determined 20 polycyclic aromatic hydrocarbons (PAHs) and 12 polychlorinated biphenyls (PCBs) in Oi, Oe, and Oa horizons and at 0-5 and 15-20 cm mineral soil depth of 16 Norway spruce (Picea abies) stands in north Bavaria. The sum of PAH concentrations increased along the line Oi (mean+/-SD: 841+/-330 microg kg(-1))相似文献   
5.
In soils of the Moscow region, we examined PCB concentrations in bulk samples and aggregate fractions. Topsoils under grassland and forest at five locations along a southeast-bound transect from Moscow and at a northeastern background location (grassland only) were analysed. We collected aggregates >1 cm and fractionated them into interior and exterior portions and also analysed the remaining soil without the aggregates >1 cm. The concentrations of the sum of 17 PCBs (sigma17PCBs) in 35 bulk soil samples ranged from 3.1 to 42 microg kg(-1). This was 48-61% of the sigma33PCBs determined in 23 selected samples. The congeners 138(+158), 101 and 52 were most abundant. All PCB concentrations and the degree of chlorination declined with increasing distance from Moscow. The PCBs were accumulated in the aggregate exterior (on average 146% of the sigma17PCBs in bulk soil). We conclude that the ecotoxicological risk of PCBs in soils may not be properly assessed with the conventional bulk soil analysis.  相似文献   
6.
7.
Before wood ash can be safely used as a fertilizer in forests, possible negative effects such as input of organic contaminants or remobilization of contaminants already stored in the soil must be investigated. The objective of this study was to examine the effects of wood ash application on concentrations, storage, and distribution of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) in a Swiss forest soil. In May 1998, we added 8 Mg wood ash ha(-1) to a forest soil. We determined 20 PAHs and 14 PCBs in the organic layer, in the bulk mineral soil, and in soil material taken from preferential flow paths and from the matrix before and after the wood ash application. In the control plots, the concentrations of PAHs in the organic layer indicated moderate pollution (sum of 20 PAHs: 0.8-1.6 mg kg(-1)), but sum of PCB concentrations was high (21-48 microLg kg(-1)). The wood ash had high concentrations of PAHs (sum of 20 PAHs: 16.8 mg kg(-1)), but low concentrations of PCBs (sum of 14 PCBs: 3.4 microg kg(-1)). The wood ash application increased the PAH concentrations in the organic horizons up to sixfold. In contrast, PCB concentrations did not change in the Oa horizon and decreased up to one third in the Oi and Oe horizons. The decrease was probably caused by the mobilization of stored PCBs because of the high pH of the wood ash. This probably results in a higher mobility of dissolved organic matter, acting as PCB carrier. In the mineral soil, the preferential flow paths of the A horizon contained more PAHs and PCBs (+20 +/- 15% and +43 +/- 60%, respectively) than the matrix. This was particularly true for higher molecular weight compounds (molecular weight > 200 g mol(-1)). Below 50 cm depth, concentrations of PAHs and PCBs were smaller in the preferential flow paths, suggesting that in deeper depths, processes acting as sinks dominated over inputs in the preferential flow paths.  相似文献   
8.
PAH-pools in soils along a PAH-deposition gradient   总被引:13,自引:0,他引:13  
The objectives of this study are to characterize different PAH-pools (soil horizons, microsites influenced by stem flow, aggregate core and surface fractions, particle size fractions) in soils affected by depositions. Three forest soils affected by the emissions of an aluminium plant near Ziar/Central Slovakia were sampled to analyze 20 PAHs. The organic layers have high concentrations of PAHs (40-200 mg kg(-1)), decreasing as soil depth and distance from the aluminium plant increases. At the two sites nearest to the plant PAH-concentrations are higher in microsites affected by stem flow than in microsites not influenced by stem flow. They are also higher in aggregate surface fractions than in aggregate core fractions and in bulk soil samples than in aggregates. Sand- and siltsize particles contain decreasing percentages of the sum PAH-concentrations as distance from the plant increases. This microscale heterogeneity affects PAH-availability and has to be considered when assessing environmental risks.  相似文献   
9.
We determined the concentrations of 35 PCNs, 12 PCBs, and 20 PAHs in 49 urban topsoils under different land use (house garden, roadside grassland, alluvial grassland, park areas, industrial sites, agricultural sites) and in nine rural topsoils. The sums of concentrations of 35 PCNs (sigma35 PCNs) were <0.1-15.4 microg kg(-1) in urban soils and <0.1 to 0.82 microg kg(-1) in rural soils. The PCN, PCB, and PAH concentrations were highest at industrial sites and in house gardens. While rural soils receive PCNs, PCBs, and PAHs by common atmospheric deposition, there are site-specific sources of PCNs, PCBs, and PAHs for urban soils such as deposition of contaminated technogenic materials. The PCN, PCB, and PAH concentrations decreased from the central urban to the rural area. In the same order the contribution of lower chlorinated PCNs and PCBs increased because they are more volatile and subject to increased atmospheric transport. The PCNs 52+60, and 73 were more abundant in soil samples than in Halowax mixtures, indicating that combustion contributed to the PCN contamination of the soils.  相似文献   
10.
Previous research has shown that plant diversity influences N and P cycles. However, the effect of plant diversity on complete ecosystem N and P budgets has not yet been assessed. For 20 plots of artificially established grassland mixtures differing in plant diversity, we determined N and P inputs by bulk and dry deposition and N and P losses by mowing (and subsequent removal of the biomass) and leaching from April 2003 to March 2004. Total deposition of N and P was 2.3 +/- 0.1 and 0.2 +/- 0.01 g m(-2) yr(-1), respectively. Mowing was the main N and P loss. The net N and P budgets were negative (-6.3 +/- 1.1 g N and -1.9 +/- 0.2 g P m(-2) yr(-1)). For N, this included a conservative estimate of atmospheric N(2) fixation. Nitrogen losses as N(2)O were expected to be small at our study site (<0.05 g m(-2) yr(-1)). Legumes increased the removal of N with the harvest and decreased leaching of NH(4)-N and dissolved organic nitrogen (DON) from the canopy. Reduced roughness of grass-containing mixtures decreased dry deposition of N and P. Total dissolved P and NO(3)-N leaching from the canopy increased in the presence of grasses attributable to the decreased N and P demand of grass-containing mixtures. Species richness did not have an effect on any of the studied fluxes. Our results demonstrate that the N and P fluxes in managed grassland are modified by the presence or absence of particular functional plant groups and are mainly driven by the management.  相似文献   
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