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1.
The stereoselectivity of R,S-venlafaxine and its metabolites R,S-O-desmethylvenlafaxine, N-desmethylvenlafaxine, O,N-didesmethylvenlafaxine, N,N-didesmethylvenlafaxine and tridesmethylvenlafaxine was studied in three processes: (i) anaerobic and aerobic laboratory scale tests; (ii) six wastewater treatment plants (WWTPs) operating under different conditions; and (iii) a variety of wastewater treatments including conventional activated sludge, natural attenuation along a receiving river stream and storage in operational and seasonal reservoirs. In the laboratory and field studies, the degradation of the venlafaxine yielded O-desmethylvenalfaxine as the dominant metabolite under aerobic and anaerobic conditions. Venlafaxine was almost exclusively converted to O-desmethylvenlafaxine under anaerobic conditions, but only a fraction of the drug was transformed to O-desmethylvenlafaxine under aerobic conditions. Degradation of venlafaxine involved only small stereoisomeric selectivity. In contrast, the degradation of O-desmethylvenlafaxine yielded remarkable S to R enrichment under aerobic conditions but none under anaerobic conditions. Determination of venlafaxine and its metabolites in the WWTPs agreed well with the stereoselectivity observed in the laboratory studies. Our results suggest that the levels of the drug and its metabolites and the stereoisomeric enrichment of the metabolite and its parent drug can be used for source tracking and for discrimination between domestic and nondomestic wastewater pollution. This was indeed demonstrated in the investigations carried out at the Jerusalem WWTP.  相似文献   

2.
Canopy scale emissions of isoprene and monoterpenes from Amazonian rainforest were measured by eddy covariance and eddy accumulation techniques. The peak mixing ratios at about 10 m above the canopy occurred in the afternoon and were typically about 90 pptv of α-pinene and 4–5 ppbv of isoprene. α-pinene was the most abundant monoterpene in the air above the canopy comprising ≈50% of the total monoterpene mixing ratio. Measured isoprene fluxes were almost 10 times higher than α-pinene fluxes. Normalized conditions of 30°C and 1000 μmol m−2 s−1 were associated with an isoprene flux of 2.4 mg m−2 h−1 and a β-pinene flux of 0.26 mg m−2 h−1. Both fluxes were lower than values that have been specified for Amazon rainforests in global emission models. Isoprene flux correlated with a light- and temperature-dependent emission activity factor, and even better with measured sensible heat flux. The variation in the measured α-pinene fluxes, as well as the diurnal cycle of mixing ratio, suggest emissions that are dependent on both light and temperature. The light and temperature dependence can have a significant effect on the modeled diurnal cycle of monoterpene emission as well as on the total monoterpene emission.  相似文献   

3.
Transfer of bioactive organic compounds from soil to plants might represent animal and human health risks. Sewage sludge and manure are potential sources for bioactive compounds such as human- and veterinary drugs. In the present study, uptake of the anti-diabetic compound, metformin, the antibiotic agent ciprofloxacin and the anti-coccidial narasin in carrot (Daucuscarota ssp. sativus cvs. Napoli) and barley (Hordeumvulgare) were investigated. The pharmaceuticals were selected in order to cover various chemical properties, in addition to their presence in relevant environmental matrixes. The root concentration factors (RCF) found in the present study were higher than the corresponding leaf concentration factors (LCF) for the three test pharmaceuticals. The uptake of metformin was higher compared with ciprofloxacin and narasin for all plant compartments analyzed. Metformin was studied more explicitly with regard to uptake and translocation in meadow fescue (Festucapratense), three other carrot cultivars (D.carota ssp. sativus cvs. Amager, Rothild and Nutri Red), wheat cereal (Triticumaestivum) and turnip rape seed (Brassicacampestris). Uptake of metformin in meadow fescue was comparable with uptake in the four carrot cultivars (RCF 2-10, LCF approximately 1.5), uptake in wheat cereals were comparable with barley cereals (seed concentration factors, SCF, 0.02-0.04) while the accumulation in turnip rape seeds was as high as 1.5. All three pharmaceuticals produced negative effects on growth and development of carrots when grown in soil concentration of 6-10 mg kg−1 dry weight.  相似文献   

4.
The persistence and dissipation kinetics of trifloxystrobin and tebuconazole on onion were studied after application of their combination formulation at a standard and double dose of 75 + 150 and 150 + 300 g a.i. ha?1. The fungicides were extracted with acetone, cleaned-up using activated charcoal (trifloxystrobin) and neutral alumina (tebuconazole). Analysis was carried out by gas chromatograph (GC) and confirmed by gas chromatograph mass spectrometry (GC-MS). The recovery was above 80% and limit of quantification (LOQ) 0.05 mg kg?1 for both fungicides. Initial residue deposits of trifloxystrobin were 0.68 and 1.01 mg kg?1 and tebuconazole 0.673 and 1.95 mg kg?1 from standard and double dose treatments, respectively. Dissipation of the fungicides followed first-order kinetics and the half life of degradation was 6–6.6 days. Matured onion bulb (and field soil) harvested after 30 days was free from fungicide residues. These findings suggest recommended safe pre-harvest interval (PHI) of 14 and 25 days for spring onion consumption after treatment of Nativo 75 WG at the standard and double doses, respectively. Matured onion bulbs at harvest were free from fungicide residues.  相似文献   

5.
Emerging contaminants in wastewater and sewage sludge spread on agricultural soil can be transferred to the human food web directly by uptake into food crops or indirectly following uptake into forage crops. This study determined uptake and translocation of the organophosphates tris(1-chloro-2-propyl) phosphate (TCPP) (log K ow 2.59), triethyl-chloro-phosphate (TCEP) (log K ow 1.44), tributyl phosphate (TBP) (log K ow 4.0), the insect repellent N,N-diethyl toluamide (DEET) (log K ow 2.18) and the plasticiser N-butyl benzenesulfonamide (NBBS) (log K ow 2.31) in barley, wheat, oilseed rape, meadow fescue and four cultivars of carrot. All species were grown in pots of agricultural soil, freshly amended contaminants in the range of 0.6–1.0 mg/kg dry weight, in the greenhouse. The bioconcentration factors for root (RCF), leaf (LCF) and seed (SCF) were calculated as plant concentration in root, leaf or seed over measured initial soil concentration, both in dry weight. The chlorinated flame retardants (TCEP and TCPP) displayed the highest bioconcentration factors for leaf and seed but did not show the same pattern for all crop species tested. For TCEP, which has been phased out due to toxicity but is still found in sewage sludge and wastewater, LCF was 3.9 in meadow fescue and 42.3 in carrot. For TCPP, which has replaced TCEP in many products and also occurs in higher residual levels in sewage sludge and wastewater, LCF was high for meadow fescue and carrot (25.9 and 17.5, respectively). For the four cultivars of carrot tested, the RCF range for TCPP and TCEP was 10–20 and 1.7–4.6, respectively. TCPP was detected in all three types of seeds tested (SCF, 0.015–0.110). Despite that DEET and NBBS have log K ow in same range as TCPP and TCEP, generally lower bioconcentration factors were measured. Based on the high translocation of TCPP and TCEP to leaves, especially TCPP, into meadow fescue (a forage crop for livestock animals), ongoing risk assessments should be conducted to investigate the potential effects of these compounds in the food web.  相似文献   

6.
Factors and sources affecting measurement uncertainty associated with monitoring metals in airborne particulate matter (PM) were investigated as part of the Windsor, Ontario Exposure Assessment Study (WOEAS). The assessment was made using co-located duplicate samples and a comparison of two analytical approaches: ED-XRF and ICP-MS. Sampling variability was estimated using relative percent difference (RPD) of co-located duplicate samples. The comparison of ICP-MS and ED-XRF results yields very good correlations (R2 ≥ 0.7) for elements present at concentrations that pass both ICP-MS and ED-XRF detection limits (e.g. Fe, Mn, Zn, Pb and Cu). PM concentration ranges (median, sample number) of 24-h indoor PM10 and personal PM10 filters, and outdoor PM2.5 filters were determined to be 2.2–40.7 (11.0, n = 48) μg m?3, 8.0–48.3 (11.9, n = 48) μg m?3, and 17.1–42.3 (21.6, n = 18) μg m?3, respectively. The gravimetric analytical results reveal that the variations in PM mass measurements for same-day sampling are insignificant compared to temporal or spatial variations: 92%, 100% and 96% of indoor, outdoor and personal duplicate samples, respectively, pass the quality criteria (RPD ≤ 20%). Uncertainties associated with ED-XRF elemental measurements of S, Ca, Mn, Fe and Zn for 24-h filter samples are low: 78%–100% of the duplicate samples passed the quality criteria. In the case of 24-h filter samples using ICP-MS, more elements passed the quality criteria due to the lower detection limits. These were: Li, Na, K, Ca, Si, Al, V, Fe, Mn, Co, Cu, Mo, Ag, Zn, Pb, As, Mg, Sb, Sn, Sr, Th, Ti, Tl, and U. Low air concentrations of metals (near or below instrumental detection limits) and/or inadvertent introduction of metal contamination are the main causes for excluding elements based on the pass/fail criteria. Uncertainty associated with elemental measurements must be assessed on an element-by-element basis.  相似文献   

7.
Wen Y  Su LM  Qin WC  Fu L  He J  Zhao YH 《Chemosphere》2012,86(6):634-640
The hydrophobic parameter represented by the octanol/water partition coefficient (log P) is commonly used to predict the soil sorption coefficient (Koc). However, a simple non-linear relationship between log Koc and log P has not been reported in the literature. In the present paper, soil sorption data for 701 compounds was investigated. The results show that log Koc is linearly related to log P for compounds with log P in the range of 0.5-7.5 and non-linearly related to log P for the compounds in a wide range of log P. A non-linear model has been developed between log Koc and log P for a wide range of compounds in the training set. This model was validated in terms of average error (AE), average absolute error (AAE) and root-mean squared error (RMSE) by using an external test set with 107 compounds. Nearly the same predictive capacity was observed in comparison with existing models. However, this non-linear model is simple, and uses only one parameter. The best model developed in this paper is a non-linear model with six correction factors for six specific classes of compounds. This model can well predict log Koc for 701 diverse compounds with AAE = 0.37. The reasons for systemic deviations in these groups may be attributed to the difference of sorption mechanism for hydrophilic/polar compounds, low solubility for highly hydrophobic compounds, hydrolysis of esters in solution, volatilization for volatile compounds and highly experimental errors for compounds with extremely high or low sorption coefficients.  相似文献   

8.
To interpret the distribution of hexabromocyclododecanes (HBCDs) in various organisms, we measured the concentrations and diastereomer and enantiomer profiles of HBCDs in 21 different species of limnic and marine cohorts from Tianjin, China. The concentration ranges of HBCDs in limnic and marine organisms were 64.3–1111 ng g−1 lw and 85.5–989 ng g−1 lw, respectively. Living habitat and feeding habits had important impacts on HBCD diastereomer distribution. Most of the species appeared to preferentially select (+)-α-, (−)-β- and (−)-γ-HBCD. There is a tendency that the total and α-HBCDs were magnified as trophic level increased with trophic magnification factors (TMFs) around 2. The concentrations of HBCDs in the limnic and marine fishes were highest in the liver, followed by the gill, skin, and muscle. In terrestrial plants, the highest concentrations of HBCDs were observed in the leaf, followed by the root and the rhizosphere soil. Plants showed enantioselectivity for HBCD enantiomers, which varied with plant species and organs (leaf vs. root) of the same plant. Higher estimated daily intakes (EDIs) of HBCDs were observed from fish than from wheat.  相似文献   

9.
Isocyanatocyclohexane and isothiocyanatocyclohexane are becoming relevant compounds in urban and industrial air, as they are used in important amounts in automobile industry and building insulation, as well as in the manufacture of foams, rubber, paints and varnishes. Glass multi-sorbent tubes (Carbotrap, Carbopack, Carboxen) were connected to LCMA-UPC pump samplers for the retention of iso- and isothiocyanatocyclohexanes. The analysis was performed by automatic thermal desorption (ATD) coupled with capillary gas chromatography (GC)/mass spectrometry detector (MSD). TD-GC/MS was chosen as analytical method due to its versatility and the possibility of analysis of a wide range of volatility and polarity VOC in air samples. The method was satisfactory sensitive, selective and reproducible for the studied compounds. The concentrations of iso- and isothioisocyanatocyclohexanes were evaluated in different urban, residential and industrial locations from extensive VOC air quality and odour episode studies in several cities in the Northeastern edge of Spain. Around 200–300 VOC were determined qualitatively in each sample. Higher values of iso- and isothiocyanatocyclohexane were found in industrial areas than in urban or residential locations. The concentrations ranged between n.d.−246 and n.d.−29 μg m−3 for isocyanatocyclohexane and isothiocyanatocyclohexane, respectively, for industrial areas. On the other hand, urban and residential locations showed concentrations ranging between n.d.−164 and n.d.−29 μg m−3 for isocyanatocyclohexane and isothiocyanatocyclohexane, respectively. The site location (urban or industrial), the kind and nearness of possible iso- and isothiocyanatocyclohexane emission activities (industrial or building construction) and the changes of wind regimes throughout the year have been found the most important factors influencing the concentrations of these compounds in the different places.  相似文献   

10.
11.
ObjectiveThis cross-sectional study was conducted to assess the relationship between exposure to cadmium and circulating reproductive hormone levels in urban and rural male workers.Materials and MethodsUrinary cadmium, blood cadmium, luteinizing hormone (LH), follicle stimulating hormone (FSH) and testosterone were obtained from 86 non-smoking traffic policemen and 86 subjects working as roadmen in a rural area. All subjects were monitored to evaluate airborne exposure to cadmium.ResultsThe mean value of exposure to cadmium was 1.3 ng m?3 in traffic policemen, while the mean value was less than 0.5 ng m?3 in roadmen. The mean concentrations of urinary cadmium (1.4 vs. 0.9 μg g?1 creatinine; p = 0.001), blood cadmium (1.1 vs. 0.7 μg l?1; p = 0.000), FSH (2.6 vs. 3.2 μlU ml?1; p = 0.02) and LH (2.6 vs. 3.1 μlU ml?1; p = 0.03) were significantly different between traffic policemen and roadmen. No differences were found in the mean values of testosterone between the two groups. Multiple linear regression models showed associations between (a) urinary cadmium, airborne cadmium, working life, job category and consumption of water from water supply (b) blood cadmium, airborne cadmium and job category (c) the values of FSH and age, working life, job category, urinary cadmium and blood cadmium (d) the values of LH and both the age and working life.ConclusionThe above results must be confirmed by further studies, but they indicate the influence of exposure to the cadmium present in urban air on the circulating FSH, even at low doses.  相似文献   

12.
Recent reports have suggested that dietary and environmental estrogens such as organochlorine pollutants may play a role in the increased incidence of breast cancer in women and disorders of the male reproductive tract. For example, elevated levels of DDE and polychlorinated biphenyls (PCB) have been measured in women with breast cancer. However, it should also be noted that numerous environmental and dietary compounds have also been characterized as antiestrogenic and as inhibitors of mammary cancer cell growthin vitro and/orin vivo. Some of these compounds include 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) and related compounds, polynuclear aromatic hydrocarbons (PAH), other naturally-occurring TCDD receptor agonists, retinoids, phorbol esters, terpenes, fatty acids, and polysaccharides. Thus, it is possible that dietary and environmental estrogens and antiestrogens may be contra-active, and these interactions must be considered in the overall risk assessment of the potential adverse human and environmental health impacts of these chemicals.  相似文献   

13.
Two iodometric methods for the concentration and analysis of water samples containing organic oxidants were applied to rivers and wastewaters in Illinois, Delaware, and Pennsylvania. Oxidant concentrations detected were as high as 2.5 § 10−5 M; the methods were capable of detecting as little as 10−8 M. Compounds possibly responsible for the observed oxidizing activity include N-chloro compounds, organic peroxides, or quinones.  相似文献   

14.
Abstract

The aim of this investigation was to investigate the fate and translocation characteristics of saisenxin (SSX), a novel organic zinc fungicide, in the environment and tobacco plants under conventional field and laboratory conditions. A rapid and sensitive analytical technique based on high-performance liquid chromatography was used for determination of SSX, in soil samples and tobacco leaf, stem and root samples. The method had satisfactiry linearity (R2?=?0.9999) and the limits of detection and of quantitation of the target compound were 0.06 and 0.20?mg kg?1, respectively. The average recoveries were in the range of 89.74–94.24% in soil, leaf, stem and root samples, with relative standard deviations of <8%. For conventional field trials, the half-life (t1/2) of SSX was 5.9–6.5 days in soil and 4.8–5.3 days in tobacco leaves; the corresponding values under controlled laboratory conditions were extended to 7.1 and 7.6?days. The translocation factor (TF) values were in the range of 0–2.25 and 0–0.25 for foliage and root irrigation treatments, respectively. The TFs of SSX in tobacco indicated that tobacco had a high ability to transfer SSX upward.  相似文献   

15.
The aim of the current research was to systematically review and summarize the studies that evaluated the concentration of lead (Pb) and cadmium (Cd) in cow milk in different regions of Iran and to perform a meta-analysis of the findings. Moreover, the non-carcinogenic and carcinogenic risks of Pb and Cd through milk consumption in adult and child consumers were assessed. As a result of a systematic search in the international and national databases between January 2008 and October 2018, 17 reports involving 1874 samples were incorporated in our study for meta-analysis. The pooled concentrations of Pb and Cd were estimated to be 13.95 μg mL−1 (95% CI 9.72–18.11 μg mL−1) and 3.55 μg mL−1 (95% CI − 2.38–9.48 μg mL−1), respectively, which were lower than the WHO/FAO and national standard limits. The estimated weekly intake (EWI) of Pb and Cd through consuming milk was 16.65 and 7 μg day−1 for adults of 70 kg and 45 and 34 μg day−1 for children of 26 kg, respectively, which was well below the risk values set by Joint FAO/WHO Expert Committee on Food Additives (JECFA). The maximum target hazard quotient values (THQs) of Pb and Cd were 5.55E−5 and 5.55E−5 for adults and 5.55E−5 and 5.55E−5 for children, respectively, which were lower than 1 value, suggesting that Iranian consumers are not exposed to non-carcinogenic risk through consuming milk. Moreover, the incremental lifetime cancer risk (ILCR) of Pb estimated to be 2.96E−04 in adults and 1.0E−03 in children, indicating that consumers in Iran are at threshold carcinogenic risk of Pb through consuming milk (ILCR > 10−4). Therefore, planning and policy making for the sustainable reduction of these toxic metals in milk, particularly in industrial regions of Iran, are crucial.  相似文献   

16.
We implemented a program in which emission characterization is enabled through collaborations between academic, US and international non-governmental entities that focus on evaluation, dissemination, and in-use testing, of improved cookstoves. This effort resulted in a study of field and laboratory emissions from traditional and improved biofuel cookstoves. We found that field measured particulate emissions of actual cooking average three times those measured during simulated cooking in the laboratory. Emission factors are highly dependent on the care and skill of the operator and the resulting combustion; these do not appear to be accurately reproduced in laboratory settings. The single scattering albedo (SSA) of the emissions was very low in both lab and field measurements, averaging about 0.3 for lab tests and around 0.5 for field tests, indicating that the primary particles are climate warming. Over the course of three summers in Honduras, we measured field emissions from traditional cookstoves, relatively new improved cookstoves, and “broken-in” improved cookstoves. We found that well-designed improved cookstoves can significantly reduce PM and CO emission factors below traditional cookstoves. For improved stoves, the presence of a chimney generally resulted in lower emission factors but left the SSA unaffected. Traditional cookstoves had an average PM emission factor of 8.2 g kg?1 – significantly larger than previous studies. Particulate emission factors for improved cookstoves without and with chimneys averaged about 6.6 g kg?1 and 4.5 g kg?1, respectively. The elemental carbon (EC) fraction of PM varied significantly between individual tests, but averaged about 25% for each of the categories.  相似文献   

17.
Spatial distribution of arsenic (As) concentrations of irrigation water, soil and plant (rice) in a shallow tube-well (STW) command area (8 ha), and their relationship with Fe, Mn and P were studied. Arsenic concentrations of water in the 110 m long irrigation channel clearly decreased with distance from the STW point, the range being 68-136 μg L−1. Such decreasing trend was also noticed with Fe and P concentrations, but the trend for Mn concentrations was not remarkable. Concerning soil As, the concentration showed a decreasing tendency with distance from the pump. The NH4-oxalate extractable As contributed 36% of total As and this amount of As was associated with poorly crystalline Fe-oxides. Furthermore only 22% of total As was phosphate extractable so that most of the As was tightly retained by soil constituents and was not readily exchangeable by phosphate. Soil As (both total and extractable As) was significantly and positively correlated with rice grain As (0.296 ± 0.063 μg g−1, n = 56). Next to drinking water, rice could be a potential source of As exposure of the people living in the As affected areas of Bangladesh.  相似文献   

18.
Biogenic VOC emission estimates from the earth's surface are crucial input parameters in air quality models. Knowledge accumulated in the last years about BVOC source distributions and chemical compound species emission profiles in Europe as well as the demand of air quality modellers for a finer resolution in space and time of BVOC estimates have led to the set-up of new emission modelling systems. An updated fast BVOC emission modelling platform explicitly considering the seasonality of emission potentials and leaf temperature gradients in forest canopies by the semi-empirical emission module (seBVOC) will be proposed and used for estimating hourly values of chemical compound-specific emissions in Europe (33–68° north; 10° west to 40° east) in the years 1997, 2000, 2001, and 2003. Spatial resolution will be 10 km by 10 km. The database used contains latest land and forest distributions, updated foliar biomass densities, leaf area indices (LAI), and plant as well as chemical compound-specific emission potentials, if available. Meteorological input parameters for the respective years will be generated using the non-hydrostatic meteorological model MM5. Highest BVOC emissions occur in daytime hours around noon from the end of May to mid-August in the Mediterranean area and from the mid of June to the end of July in the boreal forests. Comparison of 3 BVOC model approaches will reveal that for July 2003, the European isoprene and monoterpene totals range from 1124 Gg to 1446 Gg and from 338 Gg to 1112 Gg, respectively. Small-scale deviations may be as high as ±0.6 Mg km?2 for July 2003, reflecting the current uncertainty range for BVOC estimates. Key sources of errors in inventories are still insufficiently detailed land use data for some areas and lacking chemically speciated plant-specific emission potentials in particular in boreal, south-eastern, and northern African landscapes. The hourly emissions of isoprene, speciated terpenes, and oxyVOC have been made available by the NatAir database.  相似文献   

19.
The Sarno River is nicknamed “the most polluted river in Europe”. The main goal of this study is to enhance our knowledge on the Sarno River water and sediment quality and on its environmental impact on the gulf of Naples (Tyrrhenian Sea, Central Mediterranean Sea) in order to become a useful assessment tool for the regional administrations. For these reasons, 32 selected polychlorinated biphenyls (PCBs) and aldrin, α-BHC, β-BHC, δ-BHC, γ-BHC (lindane), 4,4′-DDD, 4,4′-DDE, 4,4′-DDT, dieldrin, endosulfan I, endosulfan II, endosulfan sulphate, endrin, endrin aldehyde, heptachlor, heptachlor epoxide (isomer B) and methoxychlor were determined in the water dissolved phase (DP), suspended particulate matter (SPM) and sediments. Total concentrations of PCBs ranged from 1.4 to 24.9 ng L?1 in water (sum of DP and SPM) and from 1.01 to 42.54 ng g?1 in sediment samples. The concentrations of total organochlorine pesticides (OCPs) obtained in water (sum of DP and SPM) ranged from 0.54 to 7.32 ng L?1 and from 0.08 to 5.99 ng g?1 in sediment samples. Contaminant discharges of PCBs and OCPs into the sea were calculated in about 1,247 g day?1 (948 g day?1 of PCBs and 326 g day?1 of OCPs), showing that this river should account as one of the main contribution sources of PCBs and OCPs to the Tyrrhenian Sea.  相似文献   

20.
A region-wide data analysis on polychlorinated biphenyls (PCBs) in the sediment of the Great Lakes reveals a total accumulation of approximately 300 ± 50 tonnes, representing a >30% reduction from the 1980s. Evidence of in situ degradation of sediment PCB was found, with estimated t1/2 of 11 and 17 years, at two open water locations in Lake Ontario. The relative abundance of heavy homologs as well as para-chlorines decreases with increasing depth, while the opposite is true for medium and light homologs and ortho-chlorines. In Lake Michigan, the vertical pattern features enrichment of heavier congeners and reduction of ortho-chlorines in deeper sediment layers, opposite to the trend in Lake Ontario. PCBs decrease log-linearly with increasing latitude and longitude. Air deposition of PCBs to lake sediment decreases at about 0.077 ng cm−2 yr−1 per degree latitude (N) for the geographic region extending from the Great Lakes to within the Arctic Circle.  相似文献   

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