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1.
Chemical (polycyclic aromatic hydrocarbon - PAH and heavy metal) levels in stormwater and sediment samples collected from the London Orbital (M25) motorway drainage dry detention pond at Oxted, Surrey, UK were determined. Such chemicals are derived from vehicular combustion products and the wear and tear materials deposited onto the motorway surface. Gas chromatography-mass spectrometry (GC-MS) was used for the qualitative and quantitative determination of 16 USEPA priority PAHs in motorway drainage sediments. The GC-MS method, incorporating a solid phase extraction step, provides detection limits ranging from 0.17 to 0.41 mg kg(-1)(dry weight). Almost all of the 16 USEPA listed PAHs were detected. Phenanthrene, fluoranthene, pyrene, benzo(a)anthracene, chrysene, benzo(b)fluoranthene, benzo(a)pyrene and benzo(g,h,i)perylene (PAH numbers 5, 7, 8, 9, 10, 11, 13 and 16) were among the PAHs found at "higher" levels (ranging from 0.3-10.2 mg kg(-1), dry weight) in the sediment samples. PAH levels show little change along the motorway drainage silt trap (facility for reducing the levels of suspended particulate matter in the stormwater). PAH concentrations are considerably higher in the dry detention pond outflow interceptor. Statistical analysis showed that significant correlation coefficients (based on a t-test at the 95% confidence interval) were obtained between those PAHs found at high concentrations over all of the sampling sites. Several PAHs were dispersed beyond the treatment facility and accumulation in the sediment of the deer park resulted in levels ranging from 0.3-1.6 mg kg(-1), dry weight. These PAHs found beyond the treatment facility (in the local farm deer park) may contribute a serious health threat to farm animals or even fish in the aquatic environment. Heavy metal levels (V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Cd, Sb and Pb) of the drainage stormwater and sediments were determined by inductively coupled plasma mass spectrometry (ICP-MS), with quality control evaluation using two certified reference materials. Typical detection limits were found to be below 0.1 [micro sign]g l(-1) for stormwater and 0.005 mg kg(-1) for acid digested sediments. Raised heavy metal levels were found throughout the dry detention pond facility and only decrease when the stormwater is diluted following discharge into the river Eden. Statistical analysis also confirms that some significant correlations exist between various heavy metals and PAHs. However, no overall conclusive trend is found indicating that a particular PAH is deposited in sediment relative to a specific heavy metal/s. These results raise some serious concerns about the dispersion and accumulation of chemicals in the sediments of motorway stormwater drainage systems and the need for maintenance and clean-up of contaminated material from such systems.  相似文献   

2.
The state of contamination of tropical environments, particularly in Africa, remains a relatively under explored subject. Here, we determined polycyclic aromatic hydrocarbon (PAH) and trace metal concentrations in coastal sediment and biota samples (fish and mussels) from Togo (West Africa). In the sediments, the ∑21 PAH concentrations ranged from <4 ng g(-1) to 257 ng g(-1), averaging 92 ng g(-1). Concentration ratios of low molecular weight PAHs (2-3 rings) versus high molecular weight PAHs (≥4 rings) were always lower than 1 (ranging from 0.08 to 0.46) indicating that high molecular weight PAHs were dominant in all sediment samples, and that PAHs originated mainly from anthropogenic combustion activities. The sediments were also analyzed for major elements and a total of 15 trace metals, which were found in elevated concentrations. The calculated enrichment factor (EF) values relative to the Earth's crust show that the contamination is extremely severe for Cd (EF = 191), severe for Cr (EF = 18) and U (EF = 17.8), moderately severe for Zr (EF = 8.8), for Ni (EF = 6.8), Sr (EF = 5.9) and Ba (EF = 5.4), and moderate for V (EF = 3.6) and Zn (EF = 3.4). Sediments sampled in areas affected by the dumping of phosphorite mine tailings showed particularly high concentrations of trace metals. Overall, concentrations of both PAHs and trace metals in sediment tend to increase from the coastline to the open sea (2 km offshore). This is attributable to the increasingly finer texture of coastal sediment found offshore, which has a terrigenous origin and appears loaded with various contaminants through adsorption processes. Such high loads of trace metals were also found in the biota (fish and mussels). The ratio of measured trace metal concentrations in biota to threshold limits set by the World Health Organization herein defined as relative health factor (RHF) was high. Average RHF values in fish were highest for Se (470), As (250), Ag (97), Ni (78), Mn (63), Fe (53), Pb (36), Cd (10), and Cr (7) while lowest for Cu (0.08) and Zn (0.03). Cd and Al did not bioaccumulate in the analyzed fish species. In mussels, the RHF values were highest for Fe (9,108), As (295), Pb (276), Se (273), Mn (186), Ni (71), Ag (70), Cd (14), and Cu (4).  相似文献   

3.
Organotin compounds (OTs) were used in antifouling paints for more than four decades. However, due to their widespread intensive use and high toxicity, undesirable effects in non-target marine organisms have been detected since the early 1980s. Consequently, the International Maritime Organization banned new maritime applications of these products on January 1, 2003 and their presence on ship hulls from January 1, 2008. Although extensively studied in Europe, North America, Oceania, and Asia, environmental levels and effects of organotin contamination are still poorly known for South America. Thus, the current review aimed to present the actual status of this problem in South America by summarizing and comparing the available data in the literature. An overview of the OTs concentrations in sediment and biota and their effects, mainly imposex in marine gastropods, are presented. This work showed that in Atlantic coastal areas of South America there are “hot spots” of OTs contamination, similar to that observed in industrialized countries of Northern Hemisphere. On the other hand, the number of accomplished studies in the Pacific coast is extremely low. Despite the limitation on studies about OTs environmental levels and their related effects, the available data pointed out for a widespread TBT contamination along the South American coastal areas. Therefore, the establishment of baselines of organotin contamination in the Pacific coast and the implementation of temporal trend studies in the South American coastal areas is crucial to verify the effectiveness of local regulations and OTs global ban, and to map the most sensitive areas related to present and future antifouling impacts.  相似文献   

4.
The concentrations of 27 polycyclic aromatic hydrocarbons (PAHs) were determined in bottom sediments and starfish from Mohang Harbor (MH) in Taean peninsula, South Korea. In December 2007, crude oil washed ashore from the M/V Hebei Spirit and was subsequently cleaned up within a few months of the incident. The ecological risk, bioaccumulation factor (BAF), and composition of the 27 PAHs were examined. The PAH concentrations in the bottom sediment ranged from 24 to 366 μg/kg dried weight, and the ecological risk was determined as minimal (mERL-Q?<?1). Total PAH concentrations in Asterina pectinifera (inside seawall) and Asterias amurensis (outside seawall) were 1,226 and 1,477 μg/kg dry weight (d.w.), respectively. The total BAFs (∑BAF) for A. amurensis was 3.8 times higher than that of A. pectinifera, and the PAH concentrations of 5–6 log K OW were highest in the two starfish species. Further, PAH fingerprint analysis (nine alkyl-substituted PAHs fraction, low molecular weight (LMW)/high molecular weight (HMW), Phe/Ant, and Flu/Pyr), and principal component analysis (PCA) based on three crude oil samples from the M/V Hebei Spirit showed no remaining influence of crude oil.  相似文献   

5.
Polycyclic aromatic hydrocarbons (PAHs) are a major concern in environmental studies as many of them have been labeled as probable carcinogens by the International Agency for Research on Cancer (IARC 1983). Due to their lipophilic properties and resistance to degradation, PAHs can accumulate in organic tissue. As a consequence, alarming concentrations of these compounds have been found in many aquatic species. The European catfish (Silurus glanis) is a top food chain predator that is considered to be a reliable bio-indicator of environmental pollution. From 2009 to 2011, 54 specimens of S. glanis were captured from four different sites covering the area of the Po River basin (Northern Italy). Fish muscles were analyzed in the laboratory to determine the levels of nine PAHs, namely naphthalene, acenaphthene, fluorene, phenanthrene, anthracene, pyrene, benz[a]anthracene, chrysene, and benz[a]pyrene (BaP), which were detected by high-performance liquid chromatography (HPLC). The total average concentration of PAHs was 26.90?±?49.50 ng g?1 (min 0.60, max 275.75 ng g?1). Analysis showed that 9.20 % of the fish muscles exceeded the maximum levels of 2 ng g?1 set for BaP by European regulations (Commission Regulation (EC), 2006). Values measured for benz[a]pyrene ranged from 0.05 to 8.20 ng g?1 (mean 1.07?±?1.58 ng g?1). Chrysene and benz[a]anthracene, both considered potential human carcinogens (PAH2), were found at levels of 4.40 and 0.05 ng g?1 (mean values), respectively. The highest mean concentration was recorded for anthracene (12.92 ng g?1), which has been recently included in the list of substances of very high concern (SVHC) as reported by the European Chemicals Agency (ECHA 1–9, 2009).  相似文献   

6.
Sediments from the Patos Lagoon Estuary in Southern Brazil and sludge from incoming effluents were assessed for the distribution of polycyclic aromatic hydrocarbons (PAHs). Shallow sediments adjoining the City of Rio Grande were found to be contaminated by PAHs mainly near urban effluent discharge, as well as in the port area. Effluents clustered into four groups according to their sources (sewage, industrial, runoff, and mixed), with each demonstrating different contributions of PAHs to the estuary. There was a predominance of runoff and mixed sources. Navigation activity was the second most important source of PAHs to sediments. The PAHs ratio identified the origin of these contaminants as essentially pyrolytic. The impact of PAHs as a result of uncontrolled disposal or accidental discharge of PAH-rich residues was suggested for several points. These points were primarily near gas stations and motor workshops. In about 30% of sampled sediments, the concentration of benzo[a]pyrene surpassed the Threshold Effects Level adopted for marine environments.  相似文献   

7.
PAHs were measured in sediments and mussels (Mytilus chilensis) from Carboneros and Puerto Claro, located in Corral Bay, Valdivia. According to the ratio of phenanthrene/anthracene and fluoranthene/pyrene concentrations, these sites are medium polluted with PAHs originating mainly from pyrolytic sources. Fluoranthene was the major component measured in mussels (3.1-390 ng g(-1) dry weight) and sediments (6.9-74.1 ng g(-1) dry weight). In general, mussels were mainly exposed to the dissolved fraction of the lower molecular weight PAHs (tri- and tetra-aromatics) while the higher molecular ring systems (penta- and hexa-aromatics) were more bioavailable to sediments. Mussel PAHs content was relatively constant, with the exception of the 1999 summer season (March), when higher concentration values were found in both sites; however, PAHs residues in sediments showed a temporal variation.  相似文献   

8.
Fishers’ local ecological knowledge (LEK) is an additional tool to obtain information about cetaceans, regarding their local particularities, fishing interactions, and behavior. However, this knowledge could vary in depth of detail according to the level of interaction that fishers have with a specific species. This study investigated differences in small-scale fishers’ LEK regarding the estuarine dolphin (Sotalia guianensis) in three Brazilian northeast coastal communities where fishing is practiced in estuarine lagoons and/or coastal waters and where dolphin-watching tourism varies from incipient to important. The fishers (N?=?116) were asked about general characteristics of S. guianensis and their interactions with this dolphin during fishing activities. Compared to lagoon fishers, coastal fishers showed greater knowledge about the species but had more negative interactions with the dolphin during fishing activities. Coastal fishing not only offered the opportunity for fishers to observe a wider variety of the dolphin’s behavior, but also implied direct contact with the dolphins, as they are bycaught in coastal gillnets. Besides complementing information that could be used for the management of cetaceans, this study shows that the type of environment most used by fishers also affects the accuracy of the information they provide. When designing studies to gather information on species and/or populations with the support of fishers, special consideration should be given to local particularities such as gear and habitats used within the fishing community.  相似文献   

9.
The distribution, source, ecological risk and ecotoxicity of polycyclic aromatic hydrocarbons (PAHs) of sediments from 7 sampling sites, named as Xinyang (XY), Huainan (HN), Bengbu (BB), Xuyi (XuY), Fuyang (FY), Mengcheng (MC) and Zhengzhou (ZZ), in the Huaihe River basin, China, have been investigated. The total concentrations of 16 USEPA priority PAHs ranged from 62.9 to 2232.4 ng g?1 dry weight (d.w.) with a mean concentration of 1056.8 ng g?1 d.w. Through the assessment of ecological risk, we found that the levels of PAHs in the Huaihe River should not exert adverse biological effects. The total benzo[a]pyrene toxicity equivalent (TEQ) values calculated for samples varied from 0.01 to 194.1 ng g?1 d.w., with an average of 65.9 ng g?1. The toxicity data were accordant with the chemical analysis results in this study. HN, BB and ZZ showed the greatest pollution extent both in the chemical analysis and the study of ecotoxicological effects.  相似文献   

10.
Concentration of ten polycyclic aromatic hydrocarbon (PAH) compounds were determined in liver of four fish species from different trophic levels (Aurigequula fasciata, omnivore; Alepes djedaba, carnivore; Liza abu and Sardinella albella, phytoplanktivores). In all the species, similar distributions were observed in which pyrene predominated and followed by naphthalene and acenaphthylene. L. abu accumulated the highest concentration of ΣPAH, followed by S. albella, A. fasciata, and A. djedaba. No correlation between PAH content in fish liver and fish size has been found at the level of individual compounds, except for benzo[a]pyrene (p?r?=??0.704). Female fish exhibited significantly lower mean ΣPAH concentrations than male in all the species, except for L. abu.  相似文献   

11.
Blue mussels (Mytilus edulis) were collected from coastal areas and voes in Shetland and Orkney during March and April 1998 and from various coastal locations around mainland Scotland and from the Islands during October and December 1999. The polycyclic aromatic hydrocarbon concentration and composition (2- to 6-ring parent and branched) were determined for all samples. Additional analysis, including sensory assessment and the determination of n-alkanes and geochemical biomarkers, was also undertaken on the Shetland and Orkney mussels collected in 1998. Mussels from Shetland and Orkney exhibited a wide range of total PAH concentration (14.7 to 7,177 ng g(-1) wet weight). Those mussels collected in 1999 exhibited a narrower concentration range. The lowest value (mussels from Loch Kentra) was 8.4 ng g(-1) wet weight while the maximum concentration was 344.1 ng g(-1) wet weight and was determined in mussels from Granton East in the Firth of Forth. The PAH concentration ratios in mussels from Dury Voe (Grunna), Long Hope and Kirkwall Bay were consistent with a predominately petrogenic source for these contaminants. This was supported by both the sensory assessment and the n-alkane and triterpane profiles. Comparisons of the PAH concentrations in mussels with sediments collected from the same locations around Shetland and Orkney showed that in areas of high sediment PAH concentration the bioavailability of these contaminants was limited.  相似文献   

12.
Stormwater ponds are commonly used in residential and commercial areas to control flooding. The accumulation of urban contaminants in stormwater ponds can lead to water-quality problems including nutrient enrichment, chemical contamination, and bacterial contamination. This study presents 5 years of monitoring data assessing water quality of a residential subdivision pond and adjacent tidal creek in coastal South Carolina, USA. The stormwater pond is eutrophic, as described by elevated concentrations of chlorophyll and phosphorus, and experiences periodic cyanobacterial blooms. A maximum monthly average chlorophyll concentration of 318.75 μg/L was measured in the stormwater pond and 227.63 μg/L in the tidal creek. Fecal coliform bacteria (FCB) levels were measured in both the pond and the tidal creek that exceeded health and safety standards for safe recreational use. A maximum monthly average FCB level of 1,247 CFU/100 mL was measured in the stormwater pond and 12,850 CFU/100 mL in the tidal creek. In addition, the presence of antibiotic resistant bacteria and pathogenic bacteria were detected. Low concentrations of herbicides (atrazine and 2,4-D), a fungicide (chlorothalonil), and insecticides (pyrethroids and imidacloprid) were measured. Seasonal trends were identified, with the winter months having the lowest concentrations of chlorophyll and FCB. Statistical differences between the stormwater pond and the tidal creek were also noted within seasons. The tidal creek had higher FCB levels than the stormwater pond in the spring and summer, whereas the stormwater pond had higher chlorophyll levels than the tidal creek in the summer and fall seasons. Chlorophyll and FCB levels in the stormwater pond were significantly correlated with monthly average temperature and total rainfall. Pesticide concentrations were also significantly correlated with temperature and rainfall. Pesticide concentrations in the stormwater pond were significantly correlated with pesticide concentrations in the adjacent tidal creek. Chlorophyll and FCB levels in the tidal creek, however, were not significantly correlated with levels in the pond. While stormwater ponds are beneficial in controlling flooding, they may pose environmental and human health risks due to biological and chemical contamination. Management to reduce residential runoff may improve water quality in coastal stormwater ponds and their adjacent estuarine ecosystems.  相似文献   

13.
This study was performed to elucidate the distribution, concentration trend and possible source of polycyclic aromatic hydrocarbons (PAHs) in surface water and bed sediments of the Hungarian upper section of the Danube River and the Moson Danube branch. A total of 217 samples (water and sediments) were collected from four different sampling sites in the period of 2001–2010 and analysed for the 16 priority US Environmental Protection Agency PAHs. Concentrations of total 16 PAHs (∑PAHs) in water samples ranged from 25 to 1,208 ng/L, which were predominated by two- and three-ring PAHs. The ∑PAH concentrations in sediments ranged from 8.3 to 1,202.5 ng/g dry weight. Four-ring PAHs including fluoranthene and pyrene were the dominant species in sediment samples. A selected number of concentration ratios of specific PAH compounds were calculated to evaluate the possible sources of PAH contamination. The ratios reflected a pattern of pyrogenic input as a major source of PAHs. The levels of PAHs determined were compared with other sections of the Danube and other regions of the world.  相似文献   

14.
Daytime and nighttime PM(2.5) samples were collected between August 5 and 16, 2009 and between January 24 and February 4, 2010 in an industrial complex site (site A) and an electronic waste recycling site (site B) to determine the seasonal and diurnal variations of 19 individual polycyclic aromatic hydrocarbons (PAHs) with molecular weight 302 (MW302) including four highly carcinogenic dibenzopyrene (DBP) isomers dibenzo[a,l]pyrene (DBalP), dibenzo[a,e]pyrene (DBaeP), dibenzo[a,i]pyrene (DBaiP), and dibenzo[a,h]pyrene (DBahP). This is the first report on DBP isomers in air particles from South China. The total concentration of PAH MW302 isomers ranged from 1.65 to 3.60 ng m(-3) in summer and 3.82 to 9.81 ng m(-3) in winter. The strongest peaks in the chromatograms of the MW302 isomers were naphtha[2,1-a]pyrene (N21aP), dibenzo[j,l]fluoranthene (DBjlF), naphtha[1,2-b]fluoranthene (N12bF), naphtha[1,2-k]fluoranthene (N12kF) and dibenzo[a,e]fluoranthene (DBaeF), constituting 52.0 to 55.4% of the total MW302 isomers. All the MW302 isomers showed notable seasonal variations. Most of the MW302 isomers in site B showed distinctive diurnal variations with higher concentrations occurring in the night. Taking into account both concentration and potency equivalence factors (PEFs), the strongest carcinogen in the analyzed samples was DBaiP, and the ratios of sum carcinogenic potency of four highly carcinogenic DBP isomers to benzo[a]pyrene (BaP) was about 0.94 in winter to 1.89 in summer, indicating the importance of DBP isomers for the risk assessment. Health risk assessment indicated that on average, 1 in 100 000 residents in the two industrial sites may have an increased risk of cancer due to PAH exposure.  相似文献   

15.
The main objective of this study was to investigate the concentrations of polycyclic aromatic hydrocarbons (PAHs) in inter-tidal sediments of the Kenting coast, Taiwan, to assess the levels and origin of PAHs, and to provide useful information on the potential ecological risk of PAHs to benthic organisms. The total concentrations of 38 PAHs ranged from 0.2 to 493 ng/g dry weight. The high variation in total PAH concentrations was caused by the sand content of the sediment in the area. Compared with other coasts and bays in the world, the concentrations of PAHs in the inter-tidal surface sediment of the Kenting coast is low to moderate. Based on the sediment quality guidelines, the total PAH concentrations were below the effects range low value, indicating that the PAH levels in the Kenting area were within minimal effects ranges for benthic organisms. Principal component analysis and isomer ratios were analyzed to identify the contamination source in the inter-tidal surface sediment of the Kenting coast. The results of compounds’ pattern and origin analysis suggest that the source of PAHs in the inter-tidal surface sediment of the Kenting coast is the combustion of petroleum and biomass.  相似文献   

16.
Polycyclic aromatic hydrocarbons in some grounded coffee brands   总被引:1,自引:0,他引:1  
Potentially toxic 16 priority polycyclic aromatic hydrocarbons (PAHs) were determined in four brands of grounded coffee. Four to 13 PAHs were detected. Concentrations of total PAHs in different brands of coffee samples were in the range of 831.7–1,589.7 μg/kg. Benzo[a]pyrene (2A: probable human carcinogen) was found in Nescafe Premium whereas naphthalene (2B: possible human carcinogen) was found in all the samples of coffee.  相似文献   

17.
To document the spatial distribution and metal contamination in the coastal sediments of the Al-Khafji area in the northern part of the Saudi Arabian Gulf, 27 samples were collected for Al, V, Cr, Mn, Cu, Zn, Cd, Pb, Hg, Sr, As, Fe, Co, and Ni analysis using inductively coupled plasma-mass spectrometer (ICP-MS). The results revealed the following descending order of the metal concentrations: Sr > Fe > Al > As > Mn > Ni > V > Zn > Cr > Cu > Pb > Co > Hg > Cd. Average levels of enrichment factor of Sr, As, Hg, Cd, Ni, V, Cu, Co, and Pb were higher than 2 (218.10, 128.50, 80.94, 41.50, 12.31, 5.66, 2.95, 2.90, and 2.85, respectively) and that means the anthropogenic sources of these metals, while Al, Zn, Cr and Mn have enrichment factor less than 2, which implies natural sources. Average values of Sr, Hg, Cd, Cr, Ni, and As in the coastal sediments of Al-Khafji area were mostly higher than the values recorded from the background shale and earth crust and from those results along coasts of the Caspian Sea and the Mediterranean Sea. The highest levels of Cu in the northern part of the studied coastline might be due to Al-Khafji desalination plant, while levels of Al, Ni, Cr, Fe, Mn, Pb, and Zn in the central part may be a result of landfilling and industrial sewage. The highest levels of As, Cd, Co, Cu, Hg, and V in the southern part seem to be due to oil pollutants from Khafji Joint Operations (KJO). The higher values of Sr in the studied sediments in general and particularly in locality 7 could relate to the hypersalinity and aragonitic composition of the scleractinian corals abundant in that area.  相似文献   

18.
Polycyclic aromatic hydrocarbons (PAHs) and their health risks in surface soils (n?=?31) collected from coastal and estuarine areas of the northern Bohai and Yellow Seas (CEANBYS), China, were investigated. Total concentrations of PAHs ranged from 6.6?×?101 to 9.2?×?102?ng?g?1 dry weight, with an average of 3.1?×?102?ng?g?1 dw. The locations where greater concentrations of PAHs were observed were all near factories emitting black smoke or on the edge of the urban areas. These observations are consistent with concentrations of PAHs in soils being influenced by human activities, especially industrialization and urbanization. Concentrations of PAHs were significantly correlated with concentrations of organic carbon in soils. The patterns of relative concentrations and types of PAHs observed as well as knowledge of the potential sources were consistent with the primary sources of PAHs in soils of the CEANBYS being derived from the pyrolytic processes such as combustion of fossil fuel. The incremental lifetime cancer risks of exposing to PAHs for child, youth, and adult were 1.6?×?10?6, 1.2?×?10?6, and 1.9?×?10?6.  相似文献   

19.
Water samples were collected in the Pearl River Estuary in July 2002 and April 2003. The particulate and dissolved phase polycyclic aromatic hydrocarbons (PAHs) were determined. Total PAH concentrations in water samples were higher in April of 2003 (C (p): 4.0-39.1 ng/L or 445.1-1,089.9 ng/g; C (w): 15.9-184.2 ng/L) than in July of 2002 (C (p): 2.6-26.6 ng/L or 297.7-1,336.6 ng/g; C (w): 12.9-28.3 ng/L). It was found that 5, 6-ring PAHs enrich in the inner estuary samples and so did 3-ring PAHs in the July samples. Compositional differences in the suspended particulate matter (SPM) might be responsible for this observation. The partition coefficient (K (p)) increased with the increasing of the particular organic carbon content of suspended particles as well as the salinity of water, decreased with the increase of the total suspended particles content of samples. A linear correlation between logK (OC) and logK (OW) was found in two sampling periods. The observed values of logK (OC) exceed their predicted values derived form linear free energy relationship between logK (oc) and logK (ow), which could be attributed to the nonlinear sorption of soot-like carbons in suspended particles.  相似文献   

20.
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