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1.
Understanding the response of soil and surface waters to changes in atmospheric deposition is critical for guiding future legislation on air pollution. The Adirondack region of New York experiences among the most severe ecological impacts from acidic deposition. The region is characterized by considerable variability in atmospheric deposition, surficial and bedrock geology, hydrologic flow paths, and vegetation resulting in variability in effects of acidic deposition. In this study, an integrated biogeochemical model (PnET-BGC) was applied to 37 forest lake watersheds to assess the response of soil and surface waters of the Adirondacks to changes in atmospheric deposition at a regional scale. Model-simulated surface water chemistry was validated against data from two synoptic surveys conducted in 1984 and 2001. Results indicate that the model is able to capture the observed changes in surface water chemistry during this period. The model was further used to forecast the response of soil and surface waters to three future emission control scenarios. Results indicate that under the Clean Air Act, surface water SO4(2-) concentrations will continue to decrease at a median rate of -0.38 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.11 microeq/L-yr. More aggressive emission reductions will accelerate the rate of recovery. Under an aggressive control scenario, which represents an additional 75% reduction in SO2 emissions beyond the implementation of the Clean Air Act, surface water SO4(2-) concentrations are predicted to decrease at a median rate of -0.88 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.43 microeq/L-yr. Model predictions of several biologically relevant chemical indicators are also reported. 相似文献
2.
Between 1990 and 1999, SO4(2-) deposition in northern Sweden decreased by over 50%. To determine if a corresponding amelioration of stream acidity has occurred, we analyzed trends in anthropogenically driven episodic acidification in five streams during the same time period, using the Boreal Dilution Model (BDM) (Bishop, K. H.; Laudon, H.; Kohler, S. Water Resour. Res. 2000, 36, 1873-1884). Although there was no significant change in the annual average streamwater chemistry, the anthropogenically driven episodic acidification associated with spring flood runoff decreased by between 40% and 80%. A strong correlation between winter SO4(2-) deposition and the anthropogenic component of episodic acidification in these five streams suggests that future reductions of acid deposition will further improve the spring flood acidification situation in northern Sweden. These results argue that reduced emissions of acid precursors have generated significant improvements in the surface water chemistry during episodes associated with spring runoff in northern Sweden. 相似文献
3.
Larssen T 《Environmental science & technology》2005,39(20):7970-7979
During the past 20 years, acid deposition in Europe has decreased by more than 60%, yet still a large number of lakes and streams in southern Norway have not recovered to a water quality sufficient to support sustainable populations of trout or salmon. Long-term (30 years) monitoring data were used hereto constrain the calibration of the acidification model MAGIC to three Norwegian calibrated catchments. The model accounted for 60-80% of the variance in the year-to-year variations in concentrations of most of the major ions in streamwater. The results support the use of the lumped parameter acid neutralizing capacity (ANC) to link chemical parameters to biological response, as the calibration efficiency for ANC is considerably higher than for other biologically important parameters such as inorganic aluminum (Al(n+)) and pH. Three different scenarios for future deposition of sulfur were run: current legislation, maximum feasible reductions, and an illustrative scenario removing all anthropogenic deposition. These analyses show that much of the potential improvement in water quality has already occurred and that only limited further improvement can be expected from the current legislation. The current legislation is unlikely to produce ANC values sufficiently high to allow self-reproducing populations of trout at two of the three sites. Most of the response in water chemistry to reduced acid deposition has been rapid; the water chemical responses largely occur the same year or a few years after reduction in the input. The soil pool of exchangeable base cations depleted during 150 years of acid deposition, however, requires several centuries for replenishment. The uncertainties in future predictions come from several factors, such as future nitrogen dynamics and impacts from changes in seasalt and precipitation events. The differences in future water chemistry predicted from changed seasalt deposition or nitrogen dynamics are larger that the differences between different deposition scenarios. Hence, these factors must be included in future assessments of recovery from acidification. 相似文献
4.
Changes in lake water chemistry between 1984 and 2001 at 130 stratified random sites across the northeastern United States were studied to evaluate the population-level effects of decreases in acidic deposition. Surface-water S04(2-) concentrations decreased across the region at a median rate of -1.53 microequiv L(-1) year(-1). Calcium concentrations also decreased, with a median rate of -1.73 microequiv L(-1) year(-1). This decrease in Ca2+ retarded the recovery of surface water acid neutralizing capacity (Gran ANC), which increased at a median rate of 0.66 microequiv L(-1) year(-1). There were small increases in pH in all subregions except central New England and Maine, where the changes were not statistically significant. Median NO3- trends were not significant except in the Adirondacks, where NO3- concentrations increased at a rate of 0.53 microequiv L(-1) year(-1). A regionwide decrease in the concentration of total Al, especially in ponds with low ANC values (ANC < 25 microequiv L(-1)), was observed in the Adirondack subregion. These changes in Al were consistent with the general pattern of increasing pH and ANC. Despite the general pattern of chemical recovery, many ponds remain chronically acidic or are susceptible to episodic acidification. The continued chemical and biological recovery at sites in the northeastern United States will depend on further controls on S and N emissions. 相似文献
5.
Driscoll CT Driscoll KM Roy KM Mitchell MJ 《Environmental science & technology》2003,37(10):2036-2042
Long-term changes in the chemistry of wet deposition and lake water were investigated in the Adirondack Region of New York. Marked decreases in concentrations of SO4(2-) and H+ in wet deposition have occurred at two sites since the late 1970s. These decreases are consistent with long-term declines in emissions of sulfur dioxide (SO2) in the eastern United States. Changes in wet NO3- deposition and nitrogen oxides (NOx) emissions have been minor over the same interval. Virtually all Adirondack Lakes have shown marked decreases in concentrations of SO4(2-), which coincide with decreases in atmospheric S deposition. Concentrations of NO3- have also decreased in several Adirondack lakes. As atmospheric N deposition has not changed over this period, the mechanism contributing to this apparent increase in lake/watershed N retention is not evident. Decreases in concentrations of SO4(2-) + NO3- have resulted in increases in acid-neutralizing capacity (ANC) and pH and resulted in a shift in the speciation of monomeric Al from toxic inorganic species toward less toxic organic forms in some lakes. Nevertheless, many lakes continue to exhibit pH values and concentrations of inorganic monomeric Al that are critical to aquatic biota. Extrapolation of rates of ANC increase suggests that the time frame of chemical recovery of Adirondack Lakes will be several decades if current decreases in acidic deposition are maintained. 相似文献
6.
Laudon H Dillon PJ Eimers MC Semkin RG Jeffries DS 《Environmental science & technology》2004,38(22):6009-6015
In this study we have analyzed the hydrochemical effect of drought conditions during 311 hydrological episodes in nine headwater streams in central Ontario over the past 20 years. Acid Neutralization Capacity (ANC) was logarithmically correlated (p<0.05) to antecedent discharge in eight of the nine streams, with the largest decline in ANC occurring after low antecedent flow. In eight of the nine streams SO4(2-) was the most important driving mechanism of ANC decline, but dilution as well as organic acidity was important in several streams. No decrease in the SO4(2-) driven ANC decline was observed over the 20 year study period despite a approximately 40% reduction in SO4(2-) deposition. The strong correlation between ANC decline and low antecedent discharge demonstrates that episodic acidification during rain events is strongly associated with preceding drought conditions, especially in wetland-dominated catchments. The results have important implications for recoveryfrom acidification, especially in northern ecosystems where climate scenarios forecast that warmer and drier conditions will be more common. 相似文献
7.
Contemporary trends in the acid-base status of two acid-sensitive streams in western Maryland 总被引:1,自引:0,他引:1
Eshleman KN Kline KM Morgan RP Castro NM Negley TL 《Environmental science & technology》2008,42(1):56-61
Recovery of streamwater acid neutralizing capacity (ANC) resulting from declines in regional acid deposition was examined using contemporary (1990-2005) data from two long-term monitoring stations located on the Appalachian Plateau in western Maryland, U.S. Two computational methods were used to estimate daily, monthly, and annual fluxes and discharge-weighted concentrations of ANC, sulfate, nitrate, and base cations over the period of record, and two statistical methods were used to evaluate long-term trends in fluxes and concentrations. The methods used to estimate concentrations, as well as the statistical techniques, produced very similar results, underlining the robustness of the identified trends. We found clear evidence that streamwater sulfate concentrations have declined at an average rate of about 3 microeq L(-1) yr(-1) at the two sites due to a 34% reduction in wet atmospheric sulfur deposition. Trends in nitrate concentrations appear to be related to other watershed factors, especially forest disturbance. The best evidence of recovery is based on a doubling of ANC (from 21 to 42 microeq L(-1)) at the more acid-sensitive site over the 16-year period. A slowing, or possible reversal, in the sulfate, nitrate, and SBC trends is evident in our data and may portend a decline in the rate of--or end to--further recovery. 相似文献
8.
Acidification of Norwegian surface waters, as indicated by elevated concentrations of sulfate and a corresponding reduction in acid neutralizing capacity and pH, is a result of emission and subsequent deposition of sulfur and nitrogen compounds. Episodic sea-salt deposition during severe weather conditions may increase the effects of acidification by mobilizing more toxic aluminum during such episodes. Changes in climatic conditions may increase the frequency and strength of storms along the coast thus interacting with acidification effects on chemistry and biota. We found that the North Atlantic Oscillation (NAO) is linked to sea-salt deposition and sea-salt induced water chemistry effects in five rivers. Particularly, toxic levels of aluminum in all rivers were significantly correlated with higher NAO index values. Further, temporal trends were studied by comparing tendencies for selected statistical indices (i.e. frequency distributions) with time. The selected indices exhibited strong correlations between the NAO index, sea-salt deposition and river data such as chloride, pH and inorganic monomeric aluminum, pointing at the influence of North Atlantic climate variability on water chemistry and water toxicity. The potentially toxic effects of sea-salt deposition in rivers seem to be reduced as the acidification is reduced. This suggests that sea-salt episodes have to increase in strength in order to give the same potential negative biological effects in the future, if acid deposition is further reduced. More extreme winter precipitation events have been predicted in the northwest of Europe as a result of climate change. If this change will be associated with more severe sea-salt episodes is yet unknown. 相似文献
9.
10.
Erlandsson M Bishop K Fölster J Guhrén M Korsman T Kronnäs V Moldan F 《Environmental science & technology》2008,42(1):43-48
Two fundamentally different approaches to define reference conditions for acidification assessments are hydrogeochemical modeling and paleolimnological reconstructions. Both methods have been applied to calculate the preindustrial chemistry for 55 Swedish lakes in two independent studies. This paper investigates whether these methods give similar reconstructions of the preindustrial pH for these lakes. Special focus has been attached to the importance of total organic carbon concentrations and CO2 partial pressure (pCO2) in the conversion from ANC to pH in the hydrogeochemical modeling. With a uniform pCO2 value for all the lakes of 0.63 matm, the mean absolute difference between pH from the hydrogeochemical model and the paleolimnological pH was +0.23 units (mean absolute difference 0.36 units). If instead a lake specific preindustrial pCO2 is assumed, equal to contemporary pCO2, the mean difference in the predicted preindustrial pH between the two methods was reduced to +0.03 units (mean absolute difference 0.22 units). Statistical analyses indicated that with a lake specific pCO2, the difference between the reconstructions is smaller than 0.13 pH-units at a 95% level of significance. The results of this study build confidence in the reliability of both methods, providing that lake-specific estimates of pC02 are used. 相似文献
11.
Nitrous oxide (N(2)O) is an important greenhouse gas (GHG) which has a global warming potential 310 times that of carbon dioxide (CO(2)) over a hundred year lifespan. N(2)O is generated during microbial nitrification and denitrification, which are common in aquaculture systems. To date, few studies have been conducted to quantify N(2)O emission from aquaculture. Additionally, very little is known with respect to the microbial pathways through which N(2)O is formed in aquaculture systems. This review suggests that aquaculture can be an important anthropogenic source of N(2)O emission. The global N(2)O-N emission from aquaculture in 2009 is estimated to be 9.30 × 10(10) g, and will increase to 3.83 × 10(11)g which could account for 5.72% of anthropogenic N(2)O-N emission by 2030 if the aquaculture industry continues to increase at the present annual growth rate (about 7.10%). The possible mechanisms and various factors affecting N(2)O production are summarized, and two possible methods to minimize N(2)O emission, namely aquaponic and biofloc technology aquaculture, are also discussed. The paper concludes with future research directions. 相似文献
12.
Modeling mercury in power plant plumes 总被引:2,自引:0,他引:2
Measurements of speciated mercury (Hg) downwind of coal-fired power plants suggest that the Hg(II)/(Hg0 + HgII) ratio (where HgII is divalent gaseous Hg and Hg0 is elemental Hg) decreases significantly between the point of emission and the downwind ground-level measurement site, but that the SO2/(Hg0 + HgII) ratio is conserved. We simulated nine power plant plume events with the Reactive & Optics Model of Emissions (ROME), a reactive plume model that includes a comprehensive treatment of plume dispersion, transformation, and deposition. The model simulations fail to reproduce such a depletion in HgII. A sensitivity study of the impact of the HgII dry deposition velocity shows that a difference in dry deposition alone cannot explain the disparity. Similarly, a sensitivity study of the impact of cloud chemistry on results shows that the effect of clouds on Hg chemistry has only minimal impact. Possible explanations include HgII reduction to Hg0 in the plume, rapid reduction of HgII to Hg0 on ground surfaces, and/or an overestimation of the HgII fraction in the power plant emissions. We propose that a chemical reaction not included in current models of atmospheric mercury reduces HgII to Hg0 in coal-fired power plant plumes. The incorporation of two possible reduction pathways for HgII (pseudo-first-order decay and reaction with SO2) shows better agreement between the model simulations and the ambient measurements. These potential HgII to Hg0 reactions need to be studied in the laboratory to investigate this hypothesis. Because the speciation of Hg has a significant effect on Hg deposition, models of the fate and transport of atmospheric Hg may need to be modified to account for the reduction of HgII in coal-fired power plant plumes if such a reaction is confirmed in further experimental investigations. 相似文献
13.
The global atmospheric environment for the next generation 总被引:1,自引:0,他引:1
Dentener F Stevenson D Ellingsen K Van Noije T Schultz M Amann M Atherton C Bell N Bergmann D Bey I Bouwman L Butler T Cofala J Collins B Drevet J Doherty R Eickhout B Eskes H Fiore A Gauss M Hauglustaine D Horowitz L Isaksen IS Josse B Lawrence M Krol M Lamarque JF Montanaro V Müller JF Peuch VH Pitari G Pyle J Rast S Rodriguez I Sanderson M Savage NH Shindell D Strahan S Szopa S Sudo K Van Dingenen R Wild O Zeng G 《Environmental science & technology》2006,40(11):3586-3594
Air quality, ecosystem exposure to nitrogen deposition, and climate change are intimately coupled problems: we assess changes in the global atmospheric environment between 2000 and 2030 using 26 state-of-the-art global atmospheric chemistry models and three different emissions scenarios. The first (CLE) scenario reflects implementation of current air quality legislation around the world, while the second (MFR) represents a more optimistic case in which all currently feasible technologies are applied to achieve maximum emission reductions. We contrast these scenarios with the more pessimistic IPCC SRES A2 scenario. Ensemble simulations for the year 2000 are consistent among models and show a reasonable agreement with surface ozone, wet deposition, and NO2 satellite observations. Large parts of the world are currently exposed to high ozone concentrations and high deposition of nitrogen to ecosystems. By 2030, global surface ozone is calculated to increase globally by 1.5 +/- 1.2 ppb (CLE) and 4.3 +/- 2.2 ppb (A2), using the ensemble mean model results and associated +/-1 sigma standard deviations. Only the progressive MFR scenario will reduce ozone, by -2.3 +/- 1.1 ppb. Climate change is expected to modify surface ozone by -0.8 +/- 0.6 ppb, with larger decreases over sea than over land. Radiative forcing by ozone increases by 63 +/- 15 and 155 +/- 37 mW m(-2) for CLE and A2, respectively, and decreases by -45 +/- 15 mW m(-2) for MFR. We compute that at present 10.1% of the global natural terrestrial ecosystems are exposed to nitrogen deposition above a critical load of 1 g N m(-2) yr(-1). These percentages increase by 2030 to 15.8% (CLE), 10.5% (MFR), and 25% (A2). This study shows the importance of enforcing current worldwide air quality legislation and the major benefits of going further. Nonattainment of these air quality policy objectives, such as expressed by the SRES-A2 scenario, would further degrade the global atmospheric environment. 相似文献
14.
Conventional heat resistance data, D values, were previously established by other workers at optimal condition for spores outgrowth. However, in canned food conditions of outgrowth are generally suboptimal in term of pH, salt concentration, water activity. The combined effects of pH and NaCl level of the recovery medium for the D value and z(pH) value were studied. Spores of Bacillus cereus were heated at 95 degrees C in phosphate-citrate buffer media at pH 7. Cells were recovered at 25 degrees C in Nutrient Agar with pH ranging from 5 to 7 and 1% to 4% (w/w) NaCl concentration. For each condition D' values (decimal reduction time associated with the recovery media characteristics) were determined. The results show a major influence of the recovery pH on the D' values. This effect is characterised by the z'(pH) values, distance of recovery medium pH from optimum recovery pH* medium (6.7) which leads to a tenfold reduction time of D value. The increase of the salt concentration leads to a slight decrease of D' value. However z'(pH) values are not significantly affected by the salt concentration. A simple three parameter model describing the effects of pH and NaCl concentration of the recovery medium upon the heat resistance of spores is proposed. The interaction between pH and salt concentration is sufficiently low to be neglected by the model. 相似文献
15.
Role of soil freezing events in interannual patterns of stream chemistry at the Hubbard Brook Experimental Forest,New Hampshire 总被引:1,自引:0,他引:1
Fitzhugh RD Likens GE Driscoll CT Mitchell MJ Groffman PM Fahey TJ Hardy JP 《Environmental science & technology》2003,37(8):1575-1580
Soil freezing is a disturbance of the below ground environment, potentially resulting in increased losses of NO3- and surface water acidification. Here, we report the effects of soil freezing on interannual variation in stream chemistry at the Hubbard Brook Experimental Forest, New Hampshire. Data from 1970 to 1997 of soil frost depth, snow cover, precipitation, air temperature, and stream discharge and chemistry were used in a stepwise linear regression model to select the variables that best predicted deviations of annual stream concentrations from 4-year running averages. Variables quantifying soil freezing severity were selected as significant predictors of short-term fluctuations in stream K+, NO3-, Ca2+, and Mg2+ concentrations from 1970 to 1989, explaining 59 and 47% of the short-term variability in K+ and NO3-, respectively. Fine-root mortality and disturbance of root-soil-microbe interactions, with subsequent effects on decomposition and nutrient uptake, likely contributed to the mobilization of K+ and NO3- to streamwater following severe soil freezing events. The relationship between soil freezing and stream chemistry, however, weakened during the period 1990-1997. Because soil freezing has had inconsistent effects on stream chemistry during the period 1970-1997, it is unclear whether future changes in the frequency, duration, and depth of soil freezing events as the result of changes in the snow cover regime under a warmer climate will have significant impacts on the losses of NO3- and nutrient-base cations from temperate northern ecosystems. 相似文献
16.
Autogenerative high pressure digestion (AHPD) is a novel configuration of anaerobic digestion, in which micro-organisms produce autogenerated biogas pressures up to 90 bar with >90% CH(4)-content in a single step reactor. (1) The less than 10% CO(2)-content was postulated to be resulting from proportionally more CO(2) dissolution relative to CH(4) at increasing pressure. However, at 90 bar of total pressure Henry's law also predicts dissolution of 81% of produced CH(4). Therefore, in the present research we studied whether CO(2) can be selectively retained in solution at moderately high pressures up to 20 bar, aiming to produce high-calorific biogas with >90% methane. Experiments were performed in an 8 L closed fed-batch pressure digester fed with acetate as the substrate. Experimental results confirmed CH(4) distribution over gas and liquid phase according to Henry's law, but the CO(2)-content of the biogas was only 1-2%, at pH 7, that is, much lower than expected. By varying the ratio between acid neutralizing capacity (ANC) and total inorganic carbon (TIC(produced)) of the substrate between 0 and 1, the biogas CO(2)-content could be controlled independently of pressure. However, by decreasing the ANC relative to the TIC(produced) CO(2) accumulation in the aqueous medium caused acidification to pH 5, but remarkably, acetic acid was still converted into CH(4) at a rate comparable to neutral conditions. 相似文献
17.
18.
A three-dimensional source-oriented Eulerian air quality model is developed that can predict source contributions to the visibility reduction. Particulate matter and precursor gases from 14 different sources (crustal material, paved road dust, diesel engines, meat cooking, noncatalyst-equipped gasoline engines, catalyst-equipped gasoline engines, high-sulfur fuel, sea salt, refrigerant losses, residential production, animals, soil and fertilizer application, other anthropogenic sources, and background sources) are tracked though a mathematical simulation of emission, chemical reaction, gas-to-particle conversion, transport, and deposition. A visibility model based on Mie theory is modified to use the calculated source contributions to airborne particulate matter size and composition as well as gas-phase pollutant concentrations to quantify total source contributions to visibility impairment. The combined air quality-visibility model is applied to predict source contributions to visibility reduction in southern California for a typical air pollution episode (September 23-25, 1996). The model successfully predicts a severe visibility reduction in the eastern portion of the South Coast Air Basin where the average daytime visibility is measured to be less than 10 km. In the relatively clean coastal portion of the domain, the model successfully predicts that the average daytime visibility is greater than 65 km. Transportation-related sources directly account for approximately 50% of the visibility reduction (diesel engines approximately 15-20%, catalyst-equipped gasoline engines approximately 10-20%, noncatalyst-equipped gasoline engines approximately 3-5%, crustal and paved road dust approximately 5%) in the region with the most severe visibility impairment. Ammonia emissions from animal sources account for approximately 10-15% of the visibility reduction. 相似文献
19.
对无缝内衣常用的锦纶、锦氨包芯纱长丝进行了真空汽蒸处理,检测了纱线强力指标的变化,并研究了纱线经真空汽蒸处理后对织物手感、染色等指标的影响。结果表明,锦纶长丝在真空汽蒸处理后断裂强度、初始模量、屈服强力下降,断裂伸长率增加;锦氨包芯纱中的氨纶长丝在真空汽蒸处理后断裂强度、初始模量下降,弹性回复率变差,塑性变形率增大。面纱锦纶长丝和地纱锦氨包芯纱均经过真空汽蒸处理后的织物较轻薄,手感更加柔软、滑糯,悬垂性和透气性良好,但刚性稍差,织物的幅宽会相应增加;另外,织物的匀染性和织物的K/S值有所提高。 相似文献
20.
Role of sediment resuspension in the remobilization of particulate-phase metals from coastal sediments 总被引:4,自引:0,他引:4
Kalnejais LH Martin WR Signell RP Bothner MH 《Environmental science & technology》2007,41(7):2282-2288
The release of particulate-phase trace metals due to sediment resuspension has been investigated by combining erosion chamber experiments that apply a range of shear stresses typically encountered in coastal environments with a shear stress record simulated by a hydrodynamic model. Two sites with contrasting sediment chemistry were investigated. Sediment particles enriched in silver, copper, and lead, 4-50 times greater than the bulk surface-sediment content, were the first particles to be eroded. As the shear-stress level was increased in the chamber, the total mass eroded increased, butthe enrichment of these trace metals fell, approaching the bulk-sediment content. From the temporal distribution of shear stress generated by the hydrodynamic model for a site in Boston Harbor, resuspension fluxes were estimated. The erosion threshold of this site is exceeded during spring tides, releasing the particles enriched in trace metals into the water column. Due to the higher trace metal content and the regularity of resuspension, low-energy resuspension events (up to a shear stress of 0.2 N/m(2)) contribute up to 60% of the resuspension metal flux in an average year. The estimated annual quantity of copper and lead resuspended into the water column is higher than estimates of the total riverine flux for these metals. These results indicate that sediment resuspension is a very important mechanism for releasing metals into the water column and provide new insight into the chemical and physical processes controlling the long-term fate of trace metals in contaminated sediments. 相似文献