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11.
Long-range atmospheric transport of three toxaphene congeners across Europe. Modeling by chained single-box FATEMOD program 总被引:1,自引:1,他引:0
Jaakko Paasivirta Seija Sinkkonen Vladimir Nikiforov Fedor Kryuchkov Erkki Kolehmainen Katri Laihia Arto Valkonen Manu Lahtinen 《Environmental science and pollution research international》2009,16(2):191-205
Background, aims, and scope Since toxaphene (polychlorocamphene, polychloropinene, or strobane) mixtures were applied for massive insecticide use in the
1960s to replace the use of DDT, some of their congeners have been found at high latitudes far away from the usage areas.
Especially polychlorinated bornanes have demonstrated dominating congeners transported by air up to the Arctic areas. Environmental
fate modeling has been applied to monitor this phenomenon using parallel zones of atmosphere around the globe as interconnected
environments. These zones, shown in many meteorological maps, however, may not be the best way to configure atmospheric transport
in air trajectories. The latter could also be covered by connecting a chain of simple model boxes. We aim to study this alternative
approach by modeling the trajectory chain using catchment boxes of our FATEMOD model. Polychlorobornanes analyzed in biota
of the Barents Sea offered one case to study this modeling alternative, while toxaphene has been and partly still is used
massively at southern East Europe and around rivers flowing to the Aral Sea.
Materials and methods Pure model substances of three polychlorobornanes (toxaphene congeners P26, P50, and P62) were synthesized, their environmentally
important thermal properties measured by differential scanning calorimetry, as evaluated from literature data, and their temperature
dependences estimated by the QSPR programs VPLEST, WATSOLU, and TDLKOW. The evaluated property parameters were used to model
their atmospheric long-range transport from toxaphene heavy usage areas in Ukraine and Aral/SyrDarja/AmuDarja region areas,
through East Europe and Northern Norway (Finnmarken) to the Barents Sea. The time period used for the emission model was June
1997. Usual weather conditions in June were applied in the model, which was constructed by chaining FATEMOD model boxes of
the catchment’s areas along assumed maximal air flow trajectories. Analysis of the three chlorobornanes in toxaphene mixtures
function as a basis for the estimates of emission levels caused by its usage. High estimate (A) was taken from contents in
a Western product chlorocamphene and low estimate (B) from mean contents in Russian polychloroterpene products to achieve
modeled water concentrations. Bioaccumulation to analyzed lipid of aquatic biota at the target region was estimated by using
statistical calculation for persistent organic pollutants in literature.
Results The results from model runs A and B (high and low emission estimate) for levels in sea biota were compared to analysis results
of samples taken in August 1997 at Barents Sea. The model results (ng g−1 lw): 4–95 in lipid of planktovores and 7–150 in lipid of piscivores, were in fair agreement with the analysis results from
August 1997: 21–31 in Themisto libellula (chatka), 26–42 in Boreocadus saida (Polar cod), and 5–27 in Gadus morhua (cod) liver.
Discussion The modeling results indicate that the application of chained simple multimedia catchment boxes on predicted trajectory is
a useful method for estimation of volatile airborne persistent chemical exposures to biota in remote areas. For hazard assessment
of these pollutants, their properties, especially temperature dependences, must be estimated by a reasonable accuracy. That
can be achieved by using measurements in laboratory with pure model compounds and estimation of properties by thermodynamic
QSPR methods. The property parameters can be validated by comparing their values at an environmental temperature range with
measured or QSPR-estimated values derived by independent methods. The chained box method used for long-range air transport
modeling can be more suitable than global parallel zones modeling used earlier, provided that the main airflow trajectories
and properties of transported pollutants are predictable enough.
Conclusions Long-range air transport modeling of persistent, especially photo-resistant organic compounds using a chain of joint simple
boxes of catchment’s environments is a feasible method to predict concentrations of pollutants at the target area. This is
justified from model results compared with analytical measurements in Barents Sea biota in August 1997: three of six modeled
values were high and the other three low compared to the analysis results. The order of magnitude level was similar in both
modeled (planktovore and piscivore) and observed (chatka and polar cod) values of lipid samples. The obtained results were
too limited to firm validation but are sufficient to justify feasibility of the method, which prompts one to perform more
studies on this modeling system.
Recommendations and perspectives For assessment of the risk of environmental damages, chemical fate determination is an essential tool for chemical control,
e.g., for EU following the REACH rules. The present conclusion of applicability of the chained single-box multimedia modeling
can be validated by further studies using analyses of emissions and target biota in various other cases. To achieve useful
results, fate models built with databases having automatic steps for most calculations and outputs accessible to all chemical
control professionals are essential. Our FATEMOD program catchments at environments and compound properties listed in the
database represent a feasible tool for local, regional, and, according our present test results, for global exposure predictions.
As an extended use of model, emission estimates can be achieved by reversed modeling from analysis results of samples corresponding
to the target area.
This article is dedicated to the memory of Professor Alexander B Terentiev (who passed away in November 2006), our true friend.
With his Institute of Organo-Element Compounds, Russian Academy of Science, Moscow, he was an important main organizer of
the six joint Finnish–Russian seminars (every third year since 1989) on the field (‘Chemistry and Ecology of Organo-Element
Compounds’). He prompted us especially to search properties and environmental fates for various polyhalogen compounds. We
remember him for his friendly character and great sense of humor. 相似文献
12.
Bytnerowicz A Badea O Barbu I Fleischer P Fraczek W Gancz V Godzik B Grodzińska K Grodzki W Karnosky D Koren M Krywult M Krzan Z Longauer R Mankovska B Manning WJ McManus M Musselman RC Novotny J Popescu F Postelnicu D Prus-Głowacki W Skawiński P Skiba S Szaro R Tamas S Vasile C 《Environment international》2003,29(2-3):367-376
An international cooperative project on distribution of ozone in the Carpathian Mountains, Central Europe was conducted from 1997 to 1999. Results of that project indicated that in large parts of the Carpathian Mountains, concentrations of ozone were elevated and potentially phytotoxic to forest vegetation. That study led to the establishment of new long-term studies on ecological changes in forests and other ecosystems caused by air pollution in the Retezat Mountains, Southern Carpathians, Romania and in the Tatra Mountains, Western Carpathians on the Polish-Slovak border. Both of these important mountain ranges have the status of national parks and are Man & the Biosphere Reserves. In the Retezat Mountains, the primary research objective was to evaluate how air pollution may affect forest health and biodiversity. The main research objective in the Tatra Mountains was to evaluate responses of natural and managed Norway spruce forests to air pollution and other stresses. Ambient concentrations of ozone (O(3)), sulfur dioxide (SO(2)), nitrogen oxides (NO(x)) as well as forest health and biodiversity changes were monitored on densely distributed research sites. Initial monitoring of pollutants indicated low levels of O(3), SO(2), and NO(x) in the Retezat Mountains, while elevated levels of O(3) and high deposition of atmospheric sulfur (S) and nitrogen (N) have characterized the Tatra Mountains. In the Retezat Mountains, air pollution seems to have little effect on forest health; however, there was concern that over a long time, even low levels of pollution may affect biodiversity of this important ecosystem. In contrast, severe decline of Norway spruce has been observed in the Tatra Mountains. Although bark beetle seems to be the immediate cause of that decline, long-term elevated levels of atmospheric N and S depositions and elevated O(3) could predispose trees to insect attacks and other stresses. European and US scientists studied pollution deposition, soil and plant chemistry, O(3)-sensitive plant species, forest insects, and genetic changes in the Retezat and Tatra Mountains. Results of these investigations are presented in a GIS format to allow for a better understanding of the changes and the recommendations for effective management in these two areas. 相似文献
13.
Johan Tidblad Vladimir Kucera Farid Samie Surendra N. Das Chalothorn Bhamornsut Leong Chow Peng King Lung So Zhao Dawei Le Thi Hong Lien Hans Schollenberger Chozi V. Lungu David Simbi 《Water, Air, & Soil Pollution: Focus》2007,7(1-3):241-247
Many national exposure programmes have been performed in tropical and subtropical climates during the last 50 years. However,
ambitious programmes involving more than a few countries are scarce. In this paper a recently formed network of test sites
is described involving 12 test sites in Asia (India, Vietnam, Thailand, Malaysia and China including Hong Kong) and four test
sites in Africa (South Africa, Zambia and Zimbabwe). This effort is part of the 2001–2004 Swedish International Development
Agency (SIDA) funded Programme on Regional Air Pollution in Developing Countries (RAPIDC). Corrosion attack after one (2002–2003)
year of exposure (carbon steel, zinc, copper, limestone and paint coated steel) are presented together with environmental
data (SO2, NO2, HNO3, O3, particles, amount and pH of precipitation, temperature and relative humidity) for all the test sites. The obtained corrosion
values are substantially higher than expected for limestone, higher than expected for carbon steel and lower than expected
for zinc compared to values calculated using the best available dose–response functions. 相似文献
14.
Ungtae Kim Jagath J. Kaluarachchi Vladimir U. Smakhtin 《Journal of the American Water Resources Association》2008,44(5):1231-1247
Abstract: This work develops a methodology to project the future precipitation in large river basins under limited data and climate change while preserving the historical temporal and spatial characteristics. The computationally simple and reliable conditional generation method (CGM) is presented and applied to generate reliable monthly precipitation data in the upper Blue Nile River Basin of Ethiopia where rain‐fed agriculture is prevalent. The results showed that the temporal analysis with the CGM performs better to reproduce the historical long‐term characteristics than other methods, and the spatial analysis with the CGM reproduced the historical spatial structure accurately. A 100‐year time series analysis using the outcomes of the six general circulation models showed that precipitation changes by the 2050s (2040 through 2069) can be ?7 to 28% with a mean increase of about 11%. The seasonal results showed increasing wet conditions in all seasons with changes of mean precipitation of 5, 47, and 6% for wet, dry, and mild seasons, respectively. 相似文献
15.
16.
Stloukal P Verney V Commereuc S Rychly J Matisova-Rychlá L Pis V Koutny M 《Chemosphere》2012,88(10):1214-1219
Three commercially available biodegradable polymers, two different aromatic-aliphatic copolyesters and polylactic acid, intended for the fabrication of agricultural mulching films, in addition to other applications, were subjected to a series of tests with the aim of studying the relationship between their photooxidation and biodegradation. Photooxidation resulted in the rearrangement of polymeric chains, in the case of both copolyesters the events led to polymeric chain crosslinking and the formation of insoluble polymeric gel. The tendency was significantly more pronounced for the copolyester with the higher content of the aromatic constituent. As regards polylactic acid photochemical reactions were not accompanied by crosslinking but instead provoked chain scissions. A biodegradation experiment showed that, despite marked structural changes, the extent of photooxidation was not the decisive factor, which significantly modified the rate of biodegradation in all three materials investigated. The specific surface area of the sample specimens was shown to be more important. 相似文献
17.
Cabana H Jiwan JL Rozenberg R Elisashvili V Penninckx M Agathos SN Jones JP 《Chemosphere》2007,67(4):770-778
The biocatalytic elimination of the endocrine disrupting chemicals (EDC) nonylphenol (NP) and bisphenol A (BPA) and the personal care product ingredient triclosan (TCS) by the enzyme preparation from the white rot fungus Coriolopsis polyzona was investigated. Analysis of variance methodology showed that the pH and the temperature are statistically significant factors in the removal of NP, BPA and TCS. The elimination of NP and TCS was best at a temperature of 50 degrees C and the disappearance of BPA at 40 degrees C, whereas the most suitable pH for all three micropollutants was 5. After a 4-h treatment of the three target compounds at concentrations of 5 mg l(-1) all of the NP and BPA were eliminated. In the case of TCS, 65% was removed after either a 4 or an 8-h treatment. The utilisation of 2,2'-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) in the laccase/mediator system significantly increased the efficiency of the enzymatic treatment. The elimination of NP and BPA was directly associated with the disappearance of the estrogenic activity. Mass spectrometry analysis showed that the enzymatic treatment produced high molecular weight metabolites through a radical polymerization mechanism of NP, BPA and TCS. These oligomers were produced through the formation of C-C or C-O bonds. The polymerization of NP produced dimers, trimers, tetramers and pentamers which had molecular weights of 438, 656, 874 and 1092 amu respectively. The polymerization of BPA produced dimers, trimers and tetramers which had molecular weights of 454, 680 and 906 amu. Finally, the polymerization of TCS produced dimers, trimers and tetramers which had molecular weights of 574, 859 and 1146 amu. 相似文献
18.
New data on the vapour pressures and aqueous solubility of 1,8-dichlorooctane and 1,8-dibromooctane are reported as a function of temperature between 20 °C and 80 °C and 1 °C and 40 °C, respectively. For the vapour pressures, a static method was used during the measurements which have an estimated uncertainty between 3% and 5%. The aqueous solubilities were determined using a dynamic saturation column method and the values are accurate to within ±10%. 1,8-Dichlorooctane is more volatile than 1,8-dibromooctane in the temperature range covered (psat varies from 3 to 250 Pa and from 0.53 to 62 Pa, respectively) and is also approximately three times more soluble in water (mole fraction solubilities at 25 °C of 5.95 × 10−7 and 1.92 × 10−7, respectively). A combination of the two sets of data allowed the calculation of the Henry’s law constants and the air water partition coefficients. A simple group contribution concept was used to rationalize the data obtained. 相似文献
19.
A new type of environmental numerical models, hybrid environmental numerical models (HEMs) based on combining deterministic modeling and machine learning components, is introduced and formulated. Conceptual and practical possibilities of developing HEM, as an optimal synergetic combination of the traditional deterministic/first principles modeling (like that used for solving PDEs on the sphere representing model dynamics of global climate models) and machine learning components (like accurate and fast neural network emulations of model physics or chemistry processes), are discussed. Examples of developed HEMs (hybrid climate models and a hybrid wind–wave ocean model) illustrate the feasibility and efficiency of the new approach for modeling extremely complex multidimensional systems. 相似文献
20.
Kondrashov VV Reshetin VP Regens JL Gunter JT 《Environmental science and pollution research international》2002,9(5):333-336
Urbanization typically involves a continuous increase in motor vehicle use, resulting in congestion known as traffic jams. Idling emissions due to traffic jams combine with the complex terrain created by buildings to concentrate atmospheric pollutants in localized areas. This research simulates emissions concentrations and distributions for a congested street in Minsk, Belarus. Ground-level (up to 50-meters above the street's surface) pollutant concentrations were calculated using STAR (version 3.10) with emission factors obtained from the U.S. Environmental Protection Agency, wind speed and direction, and building location and size. Relative emissions concentrations and distributions were simulated at 1-meter and 10-meters above street level. The findings demonstrate the importance of wind speed and direction, and building size and location on emissions concentrations and distributions, with the leeward sides of buildings retaining up to 99 percent of the emitted pollutants within 1-meter of street level, and up to 77 percent 10-meters above the street. 相似文献