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1.
Residues of brominated diphenylethers (PBDEs), organochlorinated pesticides (OCPs) and polychlorinated biphenyls (PCBs) were measured in 40 eggs of little owls (Athene noctua), a terrestrial top predator from Belgium. The major organohalogens detected were PCBs (median 2,600 ng/g lipid, range 790-23 000 ng/g lipid). PCB 153,138/163, 170, 180 and 187 were the predominant congeners and constituted 71% of total sum PCBs. PBDEs were measurable in all samples, but their concentrations were much lower than for PCBs, with a range from 29-572 ng/g lipid (median 108 ng/g lipid). The most prevalent PBDE congeners in little owl egg samples were BDE 47, 99 and 153. This profile differs from the profile in marine bird species, for which BDE 47 was the dominant congener, indicating that terrestrial birds may be more exposed to higher brominated BDE congeners than marine birds. The fully brominated BDE 209 could be detected in one egg sample (17 ng/g lipid), suggesting that higher brominated BDEs may accumulate in terrestrial food chains. Brominated biphenyl (BB) 153 was determined in all egg samples, with levels ranging from 0.6 to 5.6 ng/g lipid (median 1.3 ng/g lipid). Additionally, hexabromocyclododecane (HBCD) could be identified and quantified in only two eggs at levels of 20 and 50 ng/g lipid. OCPs were present at low concentrations, suggesting a rather low contamination of the sampled environment with OCPs (median concentrations of sum DDTs: 826 ng/g lipid, sum chlordanes: 1,016 ng/g lipid, sum HCHs: 273 ng/g lipid). Hexachlorobenzene (HCB) and octachlorostyrene (OCS) were also found at low median levels of 134 and 3.4 ng/g lipid, respectively. Concentrations of most analytes were significantly higher in eggs collected from deserted nests in comparison to addled (unhatched) eggs, while eggshell thickness did not differ between deserted and addled eggs. No significant correlations were found between eggshell thickness and the analysed organohalogens.  相似文献   

2.
The present study determined concentrations and patterns of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in specimens of open sea, and Japanese coastal and inland avian species, which have been stored in the Environmental Specimen Bank of Ehime University (es-Bank), to examine the spatial trends. PBDEs and PCBs were detected in all the muscle samples analyzed, suggesting that PBDE pollution has spread even to the remote open sea areas, as in the case of PCBs. Japanese coastal and inland birds accumulated higher concentrations of PBDEs than open sea birds. In addition, higher PBDE/PCB concentration ratios were observed in Japanese coastal and inland birds than in open sea birds, indicating the input of PBDEs into the Japanese terrestrial environment. Compositions of PBDEs varied among avian species with a predominance of BDE47 or BDE153. This could be due to differences in their habitat, food habit and/or biotransformation capacity of PBDEs.  相似文献   

3.
Polychlorinated biphenyls (PCBs) and the structurally related polybrominated diphenyl ethers (PBDEs) have been associated with chronic neurotoxicity involving reduced motor activity and impaired attentiveness. Such neurobehavioral effects indicate that the central nervous system may represent an important target organ for the action of these persistent contaminants in wildlife. As a consequence, the brain of different terrestrial and aquatic birds collected in Switzerland was analysed for PCBs and PBDEs. In parallel, the same contaminants were examined in the accompanying adipose tissue. After clean-up by means of glass columns containing acidified silica, deactivated alumina and anhydrous sodium sulphate, the samples were analysed by high resolution gas chromatography/tandem mass spectrometry (HRGC-MS/MS). Median PCB concentrations in the brain (sum of PCB 28, PCB 52, PCB 101, PCB 118, PCB 138, PCB 153 and PCB 180) ranged between 13 ng g(-1) wet weight (ww) in blackbirds (Turdus merula) and 428 ng g(-1) ww in sparrow hawks (Accipiter nisus). Median PBDE concentrations in the brain (sum of BDE 28, BDE 47, BDE 99, BDE 100, BDE 153, BDE 154 and BDE 183) ranged from below the decision limit in buzzards (Buteo buteo) and blackbirds, to 14 ng g(-1) ww in sparrow hawks. After correction for the respective lipid content, higher PCB or PBDE concentrations in brain compared to adipose tissue, were found in three sparrow hawks, four buzzards and in all investigated blackbirds. These results suggest that a deficit in the neuroprotective function of the blood-brain barrier may cause unexpected levels of PCBs and PBDEs in the central nervous system.  相似文献   

4.
In the present study, concentrations and tissue distribution of polybrominated diphenyl ethers (PBDEs; IUPAC # 28, 47, 99, 100, 153, 154, 183, and 209) were examined in brain, adipose tissue, liver, muscle, and serum of birds of prey. Median SigmaPBDE levels (BDE 28-183) in the tissues of sparrowhawks ranged from 360 to 1900 ng/g lipid weight (lw), which was in general one order of magnitude higher than in the tissues of common buzzards (26-130 ng/g lw). There were no differences in PBDE congener patterns between the various tissues within individuals of a certain species. Inter-species differences in PBDE patterns and in particular the percentage of BDE 99, 100 and 153 were, however, pronounced between sparrowhawk and common buzzard. BDE 209 was detected in nearly all serum and in some liver samples, but not in any other tissues. This observation suggests that exposure to BDE 209 is low or that this congener is poorly accumulated. Passive (lipid content related) diffusion could not completely describe the PBDE tissue distribution, e.g. the lowest PBDE-load was measured in brain, a fairly lipid rich tissue.  相似文献   

5.
The brominated flame retardant decabromodiphenylether (DBDE) was analysed in wild birds to identify the most suitable species for monitoring time trends in DBDE contamination. This information was later used for the design of a 10-year trend study on DBDE in the European Union. DBDE was measured in muscle tissue, liver, and eggs from 10 terrestrial and four aquatic bird species. DBDE was detected in 47% of the terrestrial bird samples (nine species) and in 9% of the aquatic bird samples (six species). Peregrine falcon and sparrowhawk specimens were selected as most suitable species to determine temporal trends of DBDE. For sparrowhawks, no significant change in DBDE concentrations between 1973 and 2001 was found, although in later years more DBDE concentrations were above the detection limit. Peak DBDE levels measured in peregrines in 1995, were followed by a decline in concentrations until 2001. The same species were used for a trend study on hexabromocylcododecane (HBCD). Twenty-four percent of peregrine falcon eggs and 12% of sparrowhawk muscle samples demonstrated measurable HBCD residues. Three diastereomers of HBCD were analysed and the α-diastereomer was the predominant one in most samples. No clear time trends were observed for HBCD in either species. This study demonstrated that these DBDE and HBCD are bioavailable to birds of Northern Europe, although bioaccumulation seems to occur to a limited extent.  相似文献   

6.
Levels of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) were measured in paired human adipose tissue and liver samples (n=25) from Belgium. Average concentrations and standard deviation of sum PBDEs (congeners 28, 47, 99, 100, 153, 154 and 183) were 5.3+/-3.0 (range 1.4-13.2) and 3.6+/-2.1 (range 1.0-10.0)ngg(-1) lipid weight (lw) in adipose tissue and liver, respectively. These concentrations were similar to reported PBDE data from Belgium and were at the lower end of the concentration range reported elsewhere in the world. In both tissues under study, BDE 153 and BDE 47 were the most abundant PBDE congeners, contributing approximately 35% and 25% to the total PBDE content. Average concentrations and range of PCBs (sum of 23 congeners) were 490 (range 70-1130) and 380 (range 90-1140)ngg(-1)lw in adipose tissue and liver, respectively. No correlation between age and concentrations of PBDEs could be found (r=0.04), while PCB concentrations correlated significantly with age (r=0.62, p<0.01, for the sum PCBs; r=0.64, p<0.01 for PCB 153 alone). Factors, such as exposure pathways (food, dust and air), rates of bioaccumulation, metabolism and elimination, influence the concentrations of PBDEs differently than those of PCBs in humans.  相似文献   

7.
Breast milk samples from 40 first-time mothers from the Pacific Northwest of the US and Canada were analyzed for polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs). Total PBDEs (summation operator PBDEs), calculated by summing values for the 12 PBDEs congeners analyzed, ranged from 6 to 321 ppb (lipid weight) (mean=96 ppb; median=50 ppb). In approximately 40% of the women (15/40), summation operator PBDEs>100 ppb lw in their milk, and four samples had levels >250 ppb lw. PBDE 47 was the dominant congener in most samples, whereas PBDE 153 was predominant in a few (3/40). summation operator PCBs were calculated by summing values for the 82 PCB congeners analyzed, and ranged from 49 to 415 ppb (lipid weight) (mean=147 ppb; median=126 ppb). approximately 30% of the mothers (13/40) have summation operator PBDEs> summation operator PCBs in their milk samples, and approximately 65% (25/40) have BDE 47>PCB 153 in breast milk samples, with BDE 47 averaging 3-fold greater levels than PCB 153. Clearly, the lower brominated PBDEs are surpassing PCBs as a major environmental concern in North America, and are likely affecting significant portions of the populations in these regions. PBDEs have become a major persistent organic pollutant. However, there are no positive correlations between levels of summation operator PBDEs and summation operator PCBs, or between levels of PBDE 47 and PCB 153, suggesting there may be some differences in exposure pathways for PBDEs and PCBs in humans.  相似文献   

8.
Jin J  Liu W  Wang Y  Yan Tang X 《Chemosphere》2008,71(6):1043-1050
Polybrominated diphenyl ethers (PBDEs) are potentially harmful and persistent environmental pollutants. PBDEs concentrations are reported in plant, shellfish and sediment samples collected from Chinese Laizhou Bay. The summation operator(11)PBDE concentrations in plant and shellfish samples from Laizhou Bay were in the range of 70-5900ngg(-1) and 230-720ngg(-1) lipid, respectively. The summation operator(11)PBDEs concentrations in river sediment intervals samples ranged from 1.3 to 1800ng g(-1) dry weight. Pearson correlation analyses were performed on concentrations of PBDEs congeners of different sediment sample intervals. There were significant positive correlations for BDE 28 and BDE 100 (r=0.945, p<0.01), BDE 47 and BDE 99 (r=0.879, p<0.01), BDE 153 and BDE 154 (r=0.934, p<0.01), nona-BDEs and BDE 209 (r>0.934, p<0.01). BDE 209 was the predominant congener in all analyzed samples, consistent with the fact that deca-BDE technical mixtures are the dominant PBDEs product in Laizhou Bay. Data showed that PBDEs should be considered as an increasing pollution problem in the Laizhou Bay region.  相似文献   

9.
Li J  Yu H  Zhao Y  Zhang G  Wu Y 《Chemosphere》2008,73(2):182-186
The levels of polybrominated diphenyl ethers (PBDEs) in breast milk from Beijing, China, were studied. The 6 predominant PBDEs congeners (BDE47, BDE99, BDE100, BDE153, BDE154 and BDE183) in 23 pooled breast milk samples from 205 mothers living in Beijing were measured. Mean and median of SigmaPBDEs concentrations in all samples were 1.12ngg(-1) lipid and 1.07ngg(-1) lipid, respectively. The Statistical difference in SigmaPBDEs concentrations was found between urban areas (1.22ngg(-1) lipid, n=14) and rural areas (0.97ngg(-1) lipid n=9). The sum of BDE47 and BDE153 accounted for more than 70% of SigmaPBDEs in most samples. The significant correlation was found between the SigmaPBDEs in pooled samples and average of consumption of food of animal origin in the pools in urban area. However, there was no correlation was found between the SigmaPBDEs in pooled samples and average of consumption of food of animal origin in the pools in rural area of Beijing. The current study showed that the level of PBDEs in breast milk from Beijing was lower than that from South China and some developed countries such as USA and Sweden.  相似文献   

10.
Organohalogen chemicals in human blood from the United Kingdom   总被引:1,自引:0,他引:1  
Blood serum from 154 volunteers at 13 UK locations in 2003 were analysed for a range of PCBs, organochlorine pesticides and PBDEs. HCB, p,p'-DDE and p,p'-DDT and beta-HCH were the dominant organochlorine pesticides in most samples. BDEs 47, 99, 100, 153, 154 and 183 were the most regularly detected PBDEs. This study is the first report of BDE209 in UK human blood (found in 11 samples, range < 15-240 ng/g lipid). Concentration and age correlated for the less easily metabolised PCBs, p,p'-DDT and p,p'-DDE, HCB and HCHs. With increasing age females tended to have lower concentrations of the more chlorinated PCBs than males. Similar PBDE concentrations, and distributions, to those reported in the general population in Sweden in 2002 were found, despite differences in historical PBDE production and usage. There is increasing regulation to control persistent and bioaccumulative chemicals, and establishing human exposure will help to identify substances which should be urgently phased out.  相似文献   

11.
The levels of polychlorinated dibenzo-dioxins (PCDDs), polychlorinated dibenzo-furans (PCDFs), coplanar polychlorinated biphenyls (coPCBs), and polybrominated diphenyl ethers (PBDEs) were measured in fish collected from San Francisco Bay in 2000 and from the California coast in 2001. The samples were composites of only the edible portions of the fish (skin on, skin off, or whole body minus head and guts) of comparable size and from distinct geographical areas. Sixty-five composite samples were analyzed for PCDD/PCDF/coPCBs, and 43 composite samples were analyzed for PBDEs. For all fish of all species from all sampling areas, the mean concentration of the sum of BDEs 47, 99, 100, 153, and 154 was 302 ng/g lipid weight, with BDE 47>100>99 approximately 154>153. For all fish of all species from all sampling areas, the mean PCDD/PCDF International Toxic Equivalent (I-TEQ) was 33.1 pg/g lipid. For the three coPCBs (77, 126, 169), the mean I-TEQ for all fish of all species from all sampling areas was 109 pg/g lipid. The highest concentrations of both PCDD/PCDF/coPCBs and PBDEs were found in the highly populated areas of San Francisco Bay, the Los Angeles area, and San Diego Bay.  相似文献   

12.
Polybrominated diphenyl ethers (PBDEs) and organochlorine compounds (OCs) were determined in the blubber of male finless porpoises (Neophocaena phocaenoides) collected in 1990 and 2000/01 from the South China Sea. Among the organohalogen compounds analyzed, DDTs and PCBs were the predominant contaminants in the porpoises, ranging from 26,000 to 260,000 and 1400 to 28,000 ng/g lipid wt., respectively. PBDEs ranged from a minimum of 84 ng/g lipid wt., in 1990 to a maximum of 980 ng/g lipid wt., in 2001, showing a significant increase during the time period investigated. Congener profiles in finless porpoises did not shift to higher BDE congeners during these years, implying a continuous discharge of lower BDE commercial mixtures, such as PentaBDE. For OCs, HCHs concentrations decreased significantly, while others did not exhibit any significant temporal variation. Biomagnification factors (BMFs) were found to be highest for CHLs and lowest for HCB. PBDEs and PCBs had comparable BMFs, indicating a similar potential for biomagnification through the food web.  相似文献   

13.
Levels of polybrominated diphenyl ethers (PBDEs) have not previously been reported in Greenland. In this study shorthorn sculpins (Myoxocephalus scorpius) were sampled at three locations in southern Greenland; Usuk (no population), Igaliko (population 40) and Qaqortoq (population 3200). Furthermore uvak (Gadus ogac), spotted wolffish (Anarhichas minor), starry ray (Raja radiata), and blue mussels (Mytilus edulis) were collected at Usuk. Pooled samples of fish liver and blue mussel were analysed for lower brominated PBDEs (BDE-47, BDE-99, BDE-100 and BDE-153). The highest PBDE levels were found in Qaqortoq followed by Igaliko and Usuk. The measured sum PBDE concentrations in shorthorn sculpin collected at Qaqortoq, Igaliko and Usuk, were 8.2, 3.1 and 2.1 all in units of microg kg(-1) wet weight. In female and male uvak collected at Usuk PBDE levels of 7.1 and 12.0 microg kg(-1) wet weight were measured, while the concentrations were 1.2 microg kg(-1) in spotted wolffish, 1.4 microg kg(-1) in starry ray and 0.11 microg kg(-1) in blue mussels from the same locality all measured on a wet weight basis. The highest concentrations were measured in uvak, a top-predator on fish indicating that PBDEs are biomagnifying. The level of tetra-hexa BDEs is 15-24 times lower than PCB levels measured in the same samples, except for shorthorn sculpin collected at Qaqortoq, where the level of PBDEs was 40 times lower than the level of PCBs. The high concentration of PCBs relative to PBDEs in shorthorn sculpin collected at Qaqortoq signifies a local emission of PCBs, which is higher than the local emission of PBDEs.  相似文献   

14.
Human breast milk samples collected during 2003/04 in Buryatia, a Russian autonomous republic, were analyzed in order to assess human exposure to organohalogen compounds including organochlorine pesticides, polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs). When compared with available worldwide data, levels of HCB (23-880 ng/g lipid wt.), PCBs (69-680 ng/g lipid wt.), and HCHs (100-3700 ng/g lipid wt.) were relatively high, indicating elevated human exposure to these organochlorines (OCs) in Buryatia. In contrast to OCs, PBDE concentrations were low (0.46-1.7 ng/g lipid wt.). Out of 14 BDE congeners analyzed, BDE-28, BDE-47, BDE-100, BDE-153, BDE-197, and BDE-207 were detected. Estimated daily intakes (EDIs) of HCHs, HCB, CHLs, and PCBs by infants solely from human milk for 100%, 43%, 34%, and 17% of the samples, respectively, exceeded guideline thresholds. Although high EDIs raise concern for possible toxic effects of OCs, women in Buryatia are recommended to breastfeed due to numerous advantages of breastfeeding for mother and child.  相似文献   

15.
Xia C  Lam JC  Wu X  Sun L  Xie Z  Lam PK 《Chemosphere》2011,82(1):18-24
Concentrations of polybrominated diphenyl ethers (PBDEs) in yellow croakers (Pseudosciaena crocea) and silver pomfrets (Pampus argenteus) collected from nine coastal cities along the eastern China coastline were investigated. PBDE congeners with mono- to hexa-brominated substitutions were detected in the samples, indicating their ubiquitous distribution in the marine environment of China. The total PBDE concentration averaged 3.04 ng g−1 lipid wt, a level that was relatively lower than in other regions of the world, especially North America where Penta-BDE was extensively used. Geographically, the highest concentration of PBDEs was found in Xiamen, and the PBDE levels in yellow croakers were significantly higher than those in pomfrets in most of the selected cities, a pattern which may be related to the different feeding habits of the two species. The congener profiles of PBDEs were found to be different from the commonly detected pattern in fishes from other regions of the world (i.e., BDE47 > BDE99, BDE100 > BDE153, BDE154). BDE47 and BDE154 were the predominant congeners in both species, accounting for more than 60% of the total PBDE concentrations. The reasons for the relatively high proportion of BDE154 may be due to the debromination of higher brominated congeners such as BDE183 and BDE209 by these two species.  相似文献   

16.
Wurl O  Obbard JP 《Chemosphere》2005,58(7):925-933
Persistent organic pollutants (POPs) are ubiquitous pollutants in the marine environment, particular in coastal areas affected by industry and shipping traffic. POPs are known for their recalcitrance and toxicity in the environment, and there is increasing concern over their global distribution and impact upon wildlife. Marine surface sediment samples taken within 6 km of the coastline of Singapore were analyzed to determine prevailing concentrations of organochlorine pesticides (OCPs), polychlorinated biphenyl (PCBs) and polybrominated diphenyl ethers (PBDEs). Total PCB concentrations varied widely from 1.4 to 329.6 ng/g (average 73.9 ng/g), where high concentrations were detected at sample locations closest to industrial areas with intensive shipping traffic. Total DDT concentrations ranged from 2.2 to 11.9 ng/g (average 6.7 ng/g) and were lower than the concentration range of 3.3-46.2 ng/g measured for total HCH (average 18.1 ng/g). Ratios of DDT/(DDE+DDD) in sediments do not indicate recent inputs of DDT into Singapore's marine environment, but high concentrations of alpha-HCH and gamma-HCH show evidence for the usage of HCHs in Southeast Asia. Peak concentrations of cis- and trans-Chlordane were 10 ng/g. Among the PBDE congeners BDE 47, 99, and 100 only BDE 47 could be detected at a range of 3.4-13.8 ng/g (average 6.2 ng/g). The levels of OCPs, PCBs and PBDEs were compared to available data for other countries in Asia, and indicated relatively moderate levels of contamination. Peak concentrations of PCBs, HCH isomers, Chlordane, Heptachlor, Heptachlor epoxide and Dieldrin have the potential to induce ecotoxicological impacts based on levels specified in the sediment quality standards of the USEPA and Canadian Council of Ministers of the Environment.  相似文献   

17.
In this study we investigated the variation of organohalogenated compounds, such as polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), and organochlorine pesticides (OCPs), within and among clutches of a small insectivorous songbird, the great tit (Parus major), and determined whether egg laying order affects the concentrations of these compounds. PCBs were the major organohalogenated contaminants in the eggs of great tits (mean 4778 ng/g lipid weight), while PBDEs (mean 204 ng/g lipid weight) and DDTs (mean 601 ng/g lipid weight) were found at much lower concentrations. Within-clutch variability of PCBs, PBDEs, and DDTs residues in the egg samples was small (7%, 3%, and 22%, respectively) compared to among-clutch variability (93%, 97%, and 78%, respectively). The small within-clutch variability may be in part related to the small home range of great tits and low spatial heterogeneity of the contaminants. We found no laying order effects on the concentrations of PCBs, PBDEs, and DDTs. Our results show that random egg samples of great tits are suitable as a biomonitoring tool for contamination with persistent organohalogenated pollutants in terrestrial environments.  相似文献   

18.
In this study we investigated the accumulation, tissue-specific distribution and possible debromination of BDE 209 in a terrestrial songbird species, the European starling, using silastic implants as a method of exposure. BDE 209 accumulated in the blood of the exposed starlings to a mean peak concentration of 16+/-4.1 ng/ml on day 10. After this peak, there was a decline to 3.3+/-0.4 ng/ml blood at the end of the exposure period of 76 days, which suggests elimination of BDE 209. In the exposed group, the muscle concentrations (461 ng/g lipid weight [lw], 430 ng/g lw) were about twofold those in liver (269 ng/g lw, 237 ng/g lw). In addition to BDE 209, other PBDE congeners, particularly octa- and nonaBDEs, were also present in the muscle and liver, suggesting bioformation from BDE 209. To our knowledge, these results are the first indications for the debromination of BDE 209 in birds.  相似文献   

19.
In this paper, the first data on brominated flame retardants (BFRs), in particular polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) in eggs of bird species from South Africa are described (N=43). Concentrations of PBDEs were detected in all the studied species and in all the geographic areas. Highest concentrations of PBDEs were measured in bird eggs from the Vaal River, which is situated downstream of the most industrialized area in South Africa. Sum-PBDE concentrations were highest in eggs of one African sacred ibis (396 ng g(-1) lipid weight (lw)), possibly due to foraging on dumping sites. Lowest mean level of sum-PBDEs (2.3 ng g(-1) lw) was measured in cattle egrets (N=11) from Barberspan Sanctuary, a Ramsar site. The PBDE congener pattern showed large differences, reflecting different trophic levels, migratory behavior, distance to the source, and, exposure to different PBDE mixtures, among others. HBCD was detected only in four species, and highest levels were measured in one egg of African sacred ibis (71 ng g(-1) lw). In most species, levels of PBDEs were one to several orders of magnitude lower than levels of DDTs and PCBs. PBDEs correlated strongly with DDTs, PCBs and some other organochlorines (OCs), indicating the same source. The widespread occurrence of PBDEs in the South African avian species showed a strong need for further investigations of PBDEs in the Southern African environment.  相似文献   

20.
Gevao B  Muzaini S  Helaleh M 《Chemosphere》2008,71(2):242-247
Polybrominated diphenyl ether (PBDE) concentrations were measured in sewage sludge samples collected from three wastewater treatment plants in Kuwait over a six month period. PBDEs were detected in all samples analyzed and there were significant differences between the three wastewater treatment plants. The mean (and range) of summation PBDEs concentrations measured are as follows: Jahra 52.5 ng g(-1) (5.7-169.5 ng g(-1)); Reqqa, 144 ng g(-1) (32-296 ng g(-1)); Umm Haylaman, 377 ng g(-1) (23-1599 ng g(-1)). The differences in concentrations of the sum of penta congeners were consistently different at the three treatment plants with values increasing in the order: Jahra相似文献   

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