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1.
Solvents, greases, and rinse waters from routine vehicle maintenance contain heavy metals and volatile organic chemicals (VOCs). In Wisconsin, these fluids enter catch basins along with rinsing waters and are discharged to soil infiltration systems drainfields after mixing with domestic wastewaters in a septic tank. The purpose of this study was to monitor heavy metal and VOC removal and treatment in catch basins and septic tanks at four publicly-owned motor vehicle service stations (MVSS). Cadmium, chromium, and lead were found in catch basin wastewater, septic tank effluent, and septic tank sludge at concentrations ranging from 0.002–7.7 mg L?1. Lead was found in the highest concentration. The highest concentrations of metals were in septic tank sludge. Of the >50 VOCs scanned for in catch basin wastewater, septic tank effluent, and septic tank sludge samples, 29 were found in concentrations that exceeded analytical detection limits. Concentrations of detected VOCs ranged from 1.0–15,800 µg L?1 and the highest concentrations of VOCs were found in catch basin wastewater and septic tank sludge. Acetone, ethylbenzene, toluene, and xylenes were the most commonly found VOCs at all sampling locations. Thus, heavy metals and VOCs were not completely removed in catch basins and were discharged to septic tanks where removal occured possibly as these contaminants settled with solids in the sludge. The level of treatment was, however, inadequate and heavy metals and VOCs were discharged to drainfields.  相似文献   

2.
The removal of nitrilotriacetic acid (NTA) dosed to two full-scale septic tanks each connected to a single dwelling was monitored weekly over a period of 75 weeks. Nitrilotriacetic acid in the septic tank effluent was detected in samples diluted at least 25 times by a differential pulse polarographic technique. After an initial period of stabilization, concentrations of NTA in the effluent at both sites were always > 10 mg L?1. Mean five-weekly estimated removals of NTA during the last 50 weeks of the study ranged from 33 to 52%. Removal of NTA was probably by solids adsorption only as no acclimatization period or overall increase in removal during the investigation was apparent.  相似文献   

3.
The distribution and seasonal variations of petroleum residues in the Shatt al-Arab water column have been determined spectrofluorometrically. Their concentrations were found to vary between 1.7 to 35.4 μg L?1 Kuwait crude oil equivalents. The results suggested that petroleum hydrocarbons present in this river originated from diverse sources. Hydrocarbon amounts tend to be highest in winter (averaged 17.4 μg L?1) and lowest in summer (averaged 3.1 μg L?1).  相似文献   

4.
The occurence of organic priority pollutants in groundwater and surface water impacted by municipal landfill leachate was studied at the Orange County Landfill in Orange County, Florida. The results of the investigation were compared to existing data from two municipal landfills in Alachua County, Florida. The investigation in Orange County evaluated existing wells and surface water stations through sampling of groundwater, surface water, sediment, and aquatic biota. Very few organic priority pollutants were detected. The constituents most frequently found were volatile organic compounds, particularly aromatic organic constituents. Volatile organic compounds were detected in groundwater at total concentrations of less than 100 Μg L?1. Few base/neutral and acid extractable organic priority pollutants were detected. Data from the Alachua County landfills indicated the presence of volatile organic compounds in groundwater at both landfill sites but few organic priority pollutants in the base/neutral and acid extractable group were fouund. Any organic priority pollutants that were present in the solid waste as deposited were likely metabolized by microorganisms or otherwise degraded, sorbed on particulate matter, or diluted to such an extent as to be non-detected.  相似文献   

5.
Toxicity of heavy metals (Zn,Cu, Cd,Pb) to vascular plants   总被引：1，自引：0，他引：1  
The literature on heavy metal toxicity to vascular plants is reviewed. Special attention is given to forest plant species, especially trees, and effects at low metal concentrations, including growth, physiological, biochemical and cytological responses. Interactions between the metals in toxicity are considered and the role of mycorrhizal infection as well. Of the metals reviewed, Zn is the least toxic. Generally plant growth is affected at 1000 μg Zn L?1 or more in a nutrient solution, though 100 to 200 µg L?1 may give cytological disorders. At concentrations of 100 to 200 μg L?1, Cu and Cd disturb metabolic processes and growth, whereas the phytotoxicity of Pb generally is lower. Although a great variation between plant species, critical leaf tissue concentrations affecting growth in most species being 200 to 300 μg Zn g?1 dry weight, 15 to 20 μg Cu g?1 and 8–12 μg Cd g?1. With our present knowledge it is difficult to propose a limit for toxic concentrations of Zn, Cu, Cd and Pb in soils. Besides time of exposure, the degree of toxicity is influenced by biological availability of the metals and interactions with other metals in the soil, nutritional status, age and mycorrhizal infection of the plant.  相似文献   

6.
Microbial mats have been developed to sequester heavy metals from contaminated water. Mixed populations of photosynthetic and heterotrophic bacteria, dominated by Scillatoria spp., were developed for metal tolerance and integrated into a durable, self-sustaining community of microbes stimulated by and attached to ensiled grass. The mat was immobilized on glass wool and layered in flow-through baffled tanks. After allowing 8 weeks for the maturation of the mat, mixed solutions of Zn and Mn (15–16 mg L?1) were passed through a three-tank experimental series. Effluent from each tank was first sampled and then applied to the next tank. This procedure was repeated in triplicate and with six applications of new metal solution per three-tank series. By the third tank, the target metal concentration <1 mg L?1 was always achieved. Mean percentages of the initial influent concentration removed by tanks 1, 2 and 3, respectively, were 72, 93 and 98 for Zn and 78, 97 and 99 for Mn. Mean metal concentrations in the effluents (average of 6 applications) were, for tank 1: Zn (mg L?1) 5.0, Mn (mg L?1) 4.2; for tank 2: Zn 1.6, Mn 0.75; for tank 3: Zn 0.53, Mn 0.19. Mean effluent concentrations from each of the three sequential treatments (average of 6 applications per tank) were for Zn (mg L?1) 5.0, 1.6 and 0.53; for Mn (mg L?1) were 4.2, 0.75 and 0.19. Thus target concentrations were reached in experimental tank 2 for Mn and tank 3 for Zn. Metal removal in the control tank series, containing glass wool only, was 37% for Zn and 5% for Mn (average of 6 applications). Oxygen and redox potential analyses of the mat/glass wool matrix revealed a heterogenous structure of anoxic and oxic zones. Zeta potential analysis of the mat samples identified a mat surface charge ranging from ?12.3 to ?69.2 mV. Various metal removal mechanisms possibly involved with metal sequestering include surface binding to the mat or to mat exudates trapped within the glass wool, precipitation of the metals with anions present in the oxic/anoxic zones, mat mediation of the water conditions in favor of metal-oxide precipitation and active transport of the metals into the cell.  相似文献   

7.
In this report, the toxic effect of TCE (trichloroethylene), PCE (tetrachloroethylene), and potassium dichromate on P. subcapitata was investigated. The test was conducted at different concentrations of pollutants, starting from the European Community limit values defined for each analysed contaminant. Mixtures of pollutants were also tested to verify the combined effect of algae cells. Results suggest that both TCE and PCE were able to reduce P. subcapitata growth and metabolism starting from 0.05 and 0.02 mg L?1 of contaminant, respectively. PCE seems to be substantially more toxic than TCE. Chromium produces a clear effect on algae growth and esterase activity only starting from 1 mg L?1 of potassium dichromate; this result confirms the suitability of EU limit value. AFLP analysis showed that all tested pollutants produce DNA mutations probably due to oxygen radicals. Generally, chromium, at high concentrations, is more toxic and genotoxic that TCE or PCE. Test performed with a mixture of pollutants showed a synergic effect of chromium and organic compounds suggesting that the membrane damage induced from organic substances should increase the chromium cellular access.  相似文献   

8.
XIE Yue  ZHOU Li-Xiang 《土壤圈》2013,23(3):402-408
To assess the feasibility of biogenic schwertmannite to act as a sorbent for removing arsenite from groundwater, a series of biogenic schwertmannite-packed column adsorption experiments were conducted on simulated As(III)-containing groundwater. Empty bed contact time (EBCT), As(III) concentration in effluent, and the removal efficiency of As(III) through the column were investigated at pH 8.0 and temperature 25 ± 0.5 °C. The results showed that the breakthrough curves were mainly dependent on EBCT values when the influent As(III) concentration was 500 μg L-1 and the optimum EBCT was 4.0 min. When the effluent As(III) concentration reached 10 and 50 μg L-1, the breakthrough volume for the schwertmannite adsorption columns were 4 200 and 5 600 bed volume (BV), with As(III) adsorption capacity of 2.1 and 2.8 mg g-1, respectively. Biogenic schwertmannite could be regenerated by 1.0 mol L-1 NaOH solution, and more than 80% of As(III) adsorbed on the surface of schwertmannite could be released after 3 successive regenerations. The breakthrough volume for the regenerated schwertmannite-packed column still maintained 4 000--4 200 BV when the As(III) concentration in effluent was below 10 μg L-1. Compared with other sorbents for As(III) removal, the biogenic schwertmannite-packed column had a higher breakthrough volume and a much higher adsorption capacity, implying that biogenic schwertmannite was a highly efficient and potential sorbent to purify As(III)-contaminated groundwater.  相似文献   

9.
Fathead minnows (Pimephales promelas) were exposed to a range of pH and A1 concentrations in soft water (8 mg Ca L?1) to determine effect levels at various life stages. The tested pH levels ranged from 8.0 through 5.2 and inorganic monomeric Al from 15 through 60 μg L?1. Reproductive processes including spawning, embryogenesis and early larval survival were more sensitive to acid stress than were juvenile growth and survival. Juvenile survival was significantly reduced at pH 5.2 + 60 μg Al L?1 (P <0.05). Spawning success was reduced at pH 6.0 and 5.5 (P <0.10) and failed completely at pH 5.2, regardless of Al concentration. An apparant beneficial effect of added Al was observed during spawning at pH 7.5 + 35 μg Al L?1, but this effect was not significantly greater than at pH 7.5 + 15 μg Al L?1. A significant (P <0.05) decrease in larval survival occurred at pH 6.0 + 15 μg Al L?1 and lower compared to the survival at pH 7.5 + 15 μg Al L?1. Aluminum at 30 μg L?1 provided protection resulting in short term increased embryo-larval survival at pH 5.5. The effect of parental exposure on progeny survival was assessed by an interchange of embryos from the spawning treatment to all tested exposure conditions. When reared at pH 8.0 + 15 μg Al L?1 through 6.0 + 15 μg Al L?1 or at pH 5.5 + 30 μg Al L?1, parental exposure did not significantly influence progeny survival. However, survival was significantly reduced among progeny from brood fish reared at pH 5.5 + 15 μg Al L?1 as compared to those spawned at pH 6.0 + 15 μg Al L?1 and above, or at pH 5.5 + 30 μg Al L?1 (P <0.05). Juvenile or 14 d larval growth effects were not detected under any exposure condition (P >0.05). Ultimately, fathead minnow young-of-the-year recruitment and production potential can be expected to diminish when environmental pH falls to 6.0, and to fail completely at 5.5 and lower.  相似文献   

10.
A study has been conducted in a salt marsh, located in the coast of the Mar Menor lagoon (SE Spain), in which three watercourses overflow. Water samples were regularly collected over a one-year period from two transects established through the salt marsh towards the lagoon. All the samples were analysed for electrical conductivity, pH, sulphides, chlorides, nitrate, ammonium and dissolved phosphorus. The quality of the water flowing from the watercourses to the salt marsh showed a seasonal pattern, with higher contents of nitrates (> 200 mg NO? 3 L?1) in periods of maximum agricultural activities in the nearby areas, as well as a higher content of ammonium (> 30 mg NH+ 4 L?1) and phosphorus (> 10 mg PO3? 4?P L?1) when the human population increased in the zone as a result of tourism. The general spatial pattern of nutrient retention in the salt marsh, indicated by a reduction in the nutrient concentrations in the water closer to the lagoon, was modulated depending on the season. In the driest months, the marsh was 100% effective in reducing nutrient concentrations, but in the rainy periods the effectiveness was reduced. This reduction was more evident for phosphorus in autumn, whose concentration increased in the lower part of the salt marsh closer to the lagoon until it reached that of the inflow. This could mainly be explained by the accumulation of water in some sites near the lagoon, which can act as sinks of pollutants. Our data support the existence of polluted water in the surface watercourses of the area, and the associated risk can include soil salinization and the eutrophication of aquatic systems. Based on our data, the Mar Menor coastal marshes have an important role as filters to reduce pollution in this lagoon.  相似文献   

11.
Avoidance responses of an estuarine fish, mummichog (Fundulus heteroclitus), and crustacean, grass shrimp (Palaemonetes pugio) to the antifoulant his (tri-n-butyltin) oxide (TBTO) were evaluated. Four out of six groups of mummichogs tested at 1.0 μg total organic Sn L?1 showed avoidance. Total organic Sn concentrations of ≥ 3.7 μg L?1 were avoided by this fish species in all cases. Higher concentrations of total organic Sn did not result in greater avoidance responses. Grass shrimp did not avoid total organic Sn concentrations between 2.3 and 30.0 μg L?1. Response data at 2.3 and 30 μg L?1 were similar. Mummichogs and grass shrimp differed greatly in their abilities to avoid potentially adverse concentrations of total organic Sn. Since mummichogs are major predators of grass shrimp, these behavioral responses may have important implications for tidal marsh ecosystems.  相似文献   

12.
A monitoring study was carried out in an alluvial fan area in Tsukui, Central Japan during the study period of 1999–2003, in order to explain selenium (Se) behaviors in ecosystem combined with air, soil and groundwater. Monthly Se concentrations in open bulk precipitation (rainfall+aerosol, gaseous deposition and etc.), soil solution (collected by porous ceramic-cup) and groundwater ranged from 0.1 to 1.4 μg L?1 (volume-weighted average: 0.34 μg L?1), 0.21 to 1.0 μg L?1 (0.48 μg L?1) and 1.6 to 2.4 μg L?1 (2.2 μg L?1), respectively. Se concentration in open bulk precipitation was negatively correlated with the rainfall amount. Se concentration in soil solution significantly increased with DOC concentration in soil solution. Besides, despite atmospheric Se input and rainfall to the grassland study area, Se concentration in soil solution and groundwater received no significant effect from the rainfall amount, pH, Se, DOC, SO4 2?, NO3 ? and EC in rainfall. Even though Se concentrations in groundwater were significantly correlated with soil solution volume, Se, DOC and NO3 ? and groundwater level, the result of multiple regression analyses (MRA) indicated that the groundwater Se was negatively influenced by groundwater level, which depended on groundwater recharge. Se was transported into the groundwater through the groundwater recharge that largely increased in this alluvial fan study area after heavy rain.  相似文献   

13.
In the course of a series of studies conducted to investigate the long-term behavior of 129I (which has a half-life of 16 million years) in the environment, the concentration of stable iodine (127I) in precipitation, irrigation water and soil water to a depth of 2.5 m in a forest plot, an upland field and a paddy field in the upland area of Tsukuba, Japan, was determined. In the forest plot, the mean iodine concentrations in soil water at all the depths ranged from 0.13 to 0.21 μg L?1, about one-tenth of the values recorded in precipitation (weighted mean 2.1 μg L?1). This finding suggests that the major part of iodine in precipitation was sorbed onto the surface soil horizon under oxidative conditions. In the upland field, the mean iodine concentration in soil water was 2.2 μg L?1 at a depth of 0.2 m and it decreased to 0.34–0.44 μg L?1 at a depth of 0.5 m or more; these concentrations were about one-fifth of that in precipitation. This suggested that the major part of the iodine derived from precipitation was sorbed onto the subsurface soil horizon (at depths between 0.2 and 0.5 m). In the paddy field, during the non-irrigation period, the mean iodine concentrations in soil water at all the depths ranged from 1.8 to 4.8 μg L?1, almost the same values as those recorded in precipitation. During the irrigation period, the mean iodine concentrations at depths of 0.2 and 0.5 m were 18.8 and 16.7 μg L?1, values higher than the 10.9 μg L?1 value recorded in irrigation water and the 11.8 μg L?1 value recorded in ponding water. However, at a depth of 1.0 m or more, the mean iodine concentrations in soil water rapidly decreased from 7.3 to 1.8 μg L?1. These data suggested that a significant amount of iodine flowed out from the paddy field by surface runoff and a considerable amount of iodine that leached to a depth of 0.5 m was retained onto the mildly oxidative soil horizon (2Bw) that lay at depths between 0.5 and 1.0 m. At a depth of 2.5 m in the paddy field, the mean iodine concentration in soil water decreased to 1.8 μg L?1, but this level was much higher than those in the forest plot and upland field at the same depth, which suggested that a significant amount of iodine had leached into the groundwater-bearing layer. There was a negative correlation (r=-0.889) between the Eh of soil and the iodine concentration in soil water (0.2 m depth) of the paddy field. Particularly, when the Eh of soil fell below approximately 150 mV, the iodine concentration rapidly increased to above 10μg L?1. As for the chemical forms of iodine in precipitation, irrigation water, ponding water and soil water during the winter irrigation period in the paddy field with oxidative conditions, 58–82% of iodine consisted of IO? 3 and 17–42% of iodine consisted of I?. In the soil water during the summer irrigation period in the paddy field under reductive conditions, 52–58% of iodine consisted of I?, and 42–47% consisted of IO? 3.  相似文献   

14.
Phosphorus control measures at two major (>10000 people equivalent, p.e.) sewage treatment works (STWs) were installed in the lowland calcareous basin of the River Wensum (England). In-stream phosphorus concentrations were monitored seasonally from subcatchments with different levels of phosphorus impacts, as well as before and after phosphorus control, above and below the two major STWs. Point source effluents raised in-stream soluble reactive phosphorus (SRP) concentrations from 9–15 μg L?1 (agricultural sub-catchments) to 580–3270 μg L?1. This was accompanied by an increase of the SRP relative to total phosphorus from 27% to 80–90%. The phosphorus content of the suspended sediment was high (0.2 to 7.7%). Molybdate unreactive phosphorus (1–29 μg L?1) was surprisingly not affected by point source effluents. The river bed sediment bioavailable phosphorus concentrations were higher (4–18 μg g?1 wet weight) downstream from the main effluents, compared to upstream (2–6 μg g?1 wet weight). Phosphorus control at the STWs in 1999 has allowed to reduce in-stream soluble reactive concentrations to 140–280 μg L?1 but has had no significant impact on bioavailable phosphorus in the sediment by 2001, suggesting that either net sediment desorption did not occur or that it is a much slower, longer term response. The relative contribution of the diffuse sources increased from 10% to 27% of the total phosphorus loads at Fakenham. The management of these rivers is therefore problematic.  相似文献   

15.
Aluminum was added as aluminum sulfate (alum) to Lake 114, a small, shallow lake of the Experimental Lakes Area, northwestern Ontario, in spring and summer point-source additions. Aluminum and H+ gradients were established during the additions, with high Al and low pH (about 1000 μg L?1 Al, pH 4.7) near the alum sources, and background conditions (< 50 μg L?1 Al, pH 5.7) further from the sources. Approximately 80% of the added Al was lost from the water column in two weeks. Phosphorus concentrations remained unchanged during the additions, whereas lake alkalinity decreased and sulfate increased close to the sources. Dissolved organic carbon (DOC) concentrations decreased slightly (from 540 μM L?1 to about 500 μM L?1) near the alum source during the summer addition.  相似文献   

16.
Ninety-one ground water samples (predominantly from springs) in two mineralized areas of the Ouachita Mountains in west-central Arkansas, were analyzed for Fe, Mn, Zn, Cu, Co, Ni, Pb, Hg, Sb, Sr, Ba, Ca, and Li. These areas contain Mn, barite, strontianite, cinnabar, stibnite and scattered Pb-Zn mineralization, Cumulative frequency curves were used to determine the threshold and anomalous concentrations for each element in the two areas. These values were, in general, higher in the ground water from the more mineralized area for several of the base metals, but most notably for Mn and Fe, the principal metals in the Mn oxide minerals. The United States Environmental Protection Agency (EPA, 1976) criteria for Fe (300 μg L ?1) and Mn (50 μg L?1) in drinking water were exceeded, respectively, in 34% and 30% of the springs in Area I, and 13% and 23% in Area II. One spring exceeded the EPA Hg criterion (2 μg L?1) and 3 springs exceeded the 50 μg L?1 criterion for Pb. In spite of the large number of anomalous Ba concentrations, the highest concentration of Ba was 930 μg L?1 (EPA criterion 1000 μg L ?1).  相似文献   

17.
Abstract

Two separate field experiments were conducted to evaluate the effects of swine lagoon effluent relative to inorganic fertilizer at equivalent rates on phosphorus (P) status of an acidic Vaiden (very fine, montmorillonitic, thermic, Aquic Dystrudert) and an alkaline Okolona (fine, montmorillonitic, therimic, Typic Chromudert) silty clay soil. In each site, a randomized complete block design with a factorial arrangement of treatments was used. Treatments were replicated four times. Cumulative swine lagoon effluent P application rates for the year 1994 through 1996 were 0, 59, 121, and 175 kg P ha?1 on the Vaiden soil and 0, 72, 148, and 223 kg P ha?1 on the Okolona soil. In each replication, commercial fertilizer P at rates equivalent to swine effluent P application were also included. For both sites, soil P concentration increased with increasing swine effluent and commercial fertilizer P applications. No significant difference in soil P level was observed between two P sources. At high application rate, desorbed P was 1.20 and 0.59 mg P kg?1 in the Okolona and Vaiden soil respectively. In the Vaiden soil, P adsorption approached the maximum for equilibrium P concentration greater than 600 mg L?1. However, Okolona soil displayed a linear adsorption potential with application of swine effluent P. Among P fractions, NH4Cl‐P and HCl‐P concentrations increased the most compared to the check in both Okolona and Vaiden soils. Results indicated that P status differs between the soils, but no significant differences in P concentration were obtained between swine lagoon effluent and commercial fertilizer, suggesting that both P sources had similar effect on soil P after 3 years of application.  相似文献   

18.
Forest floor and mineral soil samples were collected from subalpine spruce-fir forests at 1000 m above mean sea level on 19 mountains in the northeastern United States to assess patterns in trace metal concentrations, acidity, and organic matter content. The regional average concentrations of Pb, Cu, and Zn in the forest floor were 72.3 (2.9 s.e.) μg g?1, 8.5 (0.7) μg g?1, and 46.9 (2.0) μg g?1, respectively. The regional average concentrations of Pb, Cu, and Zn in the mineral soil were 13.4 (0.8) μg g?1, and 18.2 (1.2) μg g?1, respectively. The regional average pH values of the forest floor and mineral soil were 3.99 (0.03), and 4.35 (0.03), respectively. The Green Mountains had the highest concentrations of Pb (105.7 μg g?1), and Cu (22.7 μg g?1), in the forest floor. They also had the highest concentrations of Cu (18.0 μg g?1), in the mineral soil. Site aspect did not significantly influence any of the values. Concentrations of Pb were lower than concentrations reported earlier in this decade at similar sites while concentrations of Cu and Zn remained the same. We believe that these lower Pb concentrations reflect real changes in forest Pb levels that have occurred in recent years.  相似文献   

19.
The removal and fate of runoff-derived heavy metals in a 1-yr old detention pond system were investigated during climatic conditions typical of the U.S. maritime Northwest. The catchment was a medium-sized, suburban parking lot near Portland, Oregon. Water samples from runoff, the detention pond system, and pond effluent were collected and analyzed for dissolved and particulate Cu. Copper was the dominant toxic metal for the study site, while analysis of selected samples for Pb and Cd showed these metals to be minor pollutants. Total Cu in runoff varied among different storm events over a wide range of concentrations (< 2 to 33 µg L?1), while total Cu levels in pond effluent remained within a fairly narrow range (5 to 12 µg L?1), Sediment samples collected from the detention pond system were analyzed for Cu in two size fractions (< 63 µm and < 125 µm). Copper was found to be deposited in the pond sediments in a small but highly concentrated plume (up to 130 mg kg?1), extending axially from the runoff inlet pipe. Overall, results from this study showed that low-cost, small-scale detention ponds can be a useful management practice for runoff from parking lot areas and can be of value in preserving the integrity of receiving waters.  相似文献   

20.
The relationship between the levels of CO and airborne Pb was evaluated against conditions of traffic flow, ambient air temperature and the ventilation rates in 3 underground car parks. During the study period significant variations were noted in the levels of the pollutants in each of the car parks which frequently exceeded the proposed Malaysian Air Quality Standard of 0.7 μg m?3Pb and 9 μg L?1 (8 hr average) CO for indoor environs. High correlation coefficient values were obtained between the levels of CO and traffic flow and Pb and traffic flow. High traffic flow also increased the mean air temperature inside the car parks. Reductions in the ventilation rates in the car parks caused an almost two-fold increase in the level of CO and vice versa. A simple mathematical model depicting the CO concentrations in relation to other parameters was formulated.  相似文献   

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