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1.
Zhang JB  Song CC  Yang WY 《Chemosphere》2005,59(11):1703-1705
Cold season (winter and thaw) CH4, CO2 and N2O fluxes from freshwater marshes (47°35′N, 133°31′E, Northeast China) were measured, using the static chamber method. The mean CH4 and CO2 fluxes from Carex lasiocarpa (Cl) were 0.5 ± 0.19 and 6.23 ± 1.36 mg C m−2 h−1, respectively, and those from Deyeuxia angustifoli (Da) were 0.18 ± 0.15 and 5.22 ± 2.48 mg C m−2 h−1, respectively in winter. There was no significant difference between Cl and Da (p > 0.05). The contributions of winter CH4 fluxes were about 5.5% and 3% in the Cl and Da, respectively. Marshes are an important potential N2O sink in winter season in northeast China. During thaw, the CH4 and CO2 emissions rapidly increased, 4.5–6 times of winter emissions. Wetland became a source of N2O. Cold season gases flux from northern wetlands play an important role in the seasonal gas exchange.  相似文献   

2.
Kim KH  Kim MY  Kim J 《Chemosphere》2005,59(11):1613-1624
The exchange processes of CH4 were investigated in a paddy field in the Hari area of Kang Hwa Island over an 8 day period in late April 2002. The quantification of CH4 fluxes was made under dry field condition of early spring by concurrently measuring its concentrations (at the two heights of 1 and 5 m) and the relevant micrometeorological parameters. To help elucidate the factors determining the mobilization characteristics of CH4, the results of our measurement data were examined using a number of approaches. The results of the trajectory analysis indicated that its concentration changed very sensitively with the influence of different source types, as seen from the air mass movement patterns. The concentrations and fluxes of methane, when examined over this short-term scale, showed moderately strong patterns across 24 h period in which higher values tend to occur during morning or evening. The overall results of our field measurements suggest that CH4 exchange processes in the paddy area proceeded in a fairly complicated manner. The study area behaved as a net source of CH4 to the atmosphere with a net daily emission rate of 3.6 mg m−2 despite the fact that downward deposition was observed more frequently than upward emission.  相似文献   

3.
Yacob S  Hassan MA  Shirai Y  Wakisaka M  Subash S 《Chemosphere》2005,59(11):1575-1581
Anthropogenic release of greenhouse gases, especially CO2 and CH4 has been recognized as one of the main causes of global warming. Several measures under the Kyoto Protocol 1997 have been drawn up to reduce the greenhouse gases emission. One of the measures is Clean Development Mechanisms (CDM) that was created to enable developed countries to cooperate with developing countries in emission reduction activities. In Malaysia, palm oil industry particularly from palm oil mill effluent (POME) anaerobic treatment has been identified as an important source of CH4. However, there is no study to quantify the actual CH4 emission from the commercial scale wastewater treatment facility. Hence, this paper shall address the CH4 emission from the open digesting tanks in Felda Serting Hilir Palm Oil Mill. CH4 emission pattern was recorded for 52 weeks from 3600 m3 open digesting tanks. The findings indicated that the CH4 content was between 13.5% and 49.0% which was lower than the value of 65% reported earlier. The biogas flow rate ranged between 0.8 l min−1 m−2 and 9.8 l min−1 m−2. Total CH4 emission per open digesting tank was 518.9 kg day−1. Relationships between CH4 emission and total carbon removal and POME discharged were also discussed. Fluctuation of biogas production was observed throughout the studies as a result of seasonal oil palm cropping, mill activities, variation of POME quality and quantity discharged from the mill. Thus only through long-term field measurement CH4 emission can be accurately estimated.  相似文献   

4.
Zhu R  Sun L 《Chemosphere》2005,59(11):1583-1593
Methane fluxes were measured from three exposed tundra sites and four snowpack sites on the Fildes Peninsula in the maritime Antarctic in the summertime of 2002. The average fluxes at two normal tundra sites were −15.3 μg m−2 h−1 and −14.3 μg m−2 h−1, respectively. The fluxes from tundra site with fresh penguin dropping addition showed positive values with the average of 36.1 μg m−2 h−1, suggesting that the deposition of fresh droppings greatly enhanced CH4 emissions from the poor Antarctic tundra during penguin breeding periods. The summertime variation in CH4 flux was correlated with surface ground temperature and the precipitation. The correlation between the flux and PT0, which is the product of the precipitation and surface ground temperature, was quite strong. The diurnal cycle of CH4 flux from the tundra soils was not obtained due to local fluky weather conditions. The fluxes through four snowpack sites were also obtained by the vertical CH4 concentration gradient and their average fluxes were −46.5 μg m−2 h−1, −28.2 μg m−2 h−1, −46.4 μg m−2 h−1 and −17.9 μg m−2 h−1, respectively, indicating that tundra soils under snowpack also consume atmospheric CH4 in the maritime Antarctic; therefore these fluxes could constitute an important part of the annual CH4 budget for Antarctic tundra ecosystem.  相似文献   

5.
An experiment was carried out to decompose chlorinated dioxins (PCDDs, PCDFs) Chlorobenzenes, NOx and odourous compounds (H2S, CH4S, C2H6S2, C8H8, C2H6S, C2H4O, NH3) simultaneously using a catalyst in the MSW incineration plant. The experiments were conducted at temperatures from 200°C to 400°C and from 3000h−1 to 6000h−1 at space velocity. A catalyst containing V2O5 and WO3 on the basis of TiO2 is used, an oxidizing catalyst of the honeycomb type. The average decomposition efficiencis were 95%, 98%, 92% for PCDDs(48CDDs), PCDFs(48CDFs) and Chlorobenzenes(36CLBs) at a reaction temperature of 350°C and a space velocity of 3000h−1, more than 90% for NOx at a reactiont temperature of 300°C and more than 80% for odourous compounds at the reaction temperature of 300°C and a space velocity of 6000h−1. All those compounds were decomposed successfully with increasing contact time and surface. The rate-determing step was the chemical reaction of catalyst surface.  相似文献   

6.
Wang D  He L  Shi X  Wei S  Feng X 《Chemosphere》2006,64(11):1845-1854
An investigation was conducted to estimate mercury emission to the atmosphere from different environmental surfaces and to assess its contribution to the local mercury budget in Chongqing, China. Mercury flux was measured using dynamic flux chamber (DFC) at six soil sites of three different areas (mercury polluted area, farmland and woodland) and four water surfaces from August 2003 to April 2004. The mercury emission fluxes were 3.5 ± 1.2–8.4 ± 2.5 ng m−2 h−1 for three shaded forest sites, 85.8 ± 32.4 ng m−2 h−1 for farming field, 12.3 ± 9.8–733.8 ± 255 ng m−2 h−1 for grassland sites, and 5.9 ± 12.6–618.6 ± 339 ng m−2 h−1 for water surfaces. Mercury exchange fluxes were generally higher from air/water surfaces than from air/soil surfaces. The mercury negative fluxes were found in tow soil sites at overcast days (mean = −6.4 ± 1.5 ng m−2 h−1). The diurnal and seasonal variations of mercury flux were observed in all sites. The mercury emission responded positively to the solar radiation, but negatively to the relative humidity. The mercury flux from air/soil surfaces was significantly correlated with soil temperature, which was well described by an Arrhenius-type expression with activation energy of 31.1 kcal mol−1. The annual mercury emission to the atmosphere from land surface is about 1.787 t of mercury in Chongqing.  相似文献   

7.
Gogoi N  Baruah KK  Gogoi B  Gupta PK 《Chemosphere》2005,59(11):1677-1684
Methane flux from rice varieties grown under two identical soils of Assam were monitored. In the first experiment, variety Jaya and GRT was grown in sandy loam soil of Lower Brahmaputra Valley Zone of Assam and the second experiment was conducted with variety Jyotiprasad and Bishnuprasad in sandy to sandy loam soils of Upper Brahmaputra Valley Zones of Assam. Methane flux recorded from variety Jyotiprasad and GRT was higher compared to variety Bishnuprasad and Jaya. The seasonal integrated flux recorded was 10.76 g m−2, 9.98 g m−2, 9.74 g m−2 and 11.31 g m−2 for variety GRT, Jaya, Bishnuprasad and Jyotiprasad, respectively. All the varieties exhibited two methane peaks one at maximum tillering stage and other at panicle initiation stage of the crop. Crop growth parameters such as leaf number, number of tillers and leaf area index (LAI) showed strong positive relationship with total methane flux. In both the experiments it was calculated that CH4 emission was substantially influenced by crop phenology and growth. This study emphasise the relationship of different growth parameters with methane emission.  相似文献   

8.
The temporal variability and bioaccumulation dynamics of C12–25 n-alkanes, isoprenoids and unresolved aliphatic hydrocarbons (UCM) were studied in a detritivorous fish (Sábalo: Prochilodus lineatus) collected from 1999 to 2005 in the sewage impacted Buenos Aires coastal area. Fish muscles contain huge amounts of n-C12–25 (165 ± 93, 70 ± 48 or 280 ± 134 μg g−1, dry, fresh and lipid weight, respectively) and UCM (931 ± 560, 399 ± 288 and 1567 ± 802 μg g−1) reflecting the chronic bioaccumulation of fossil fuels from sewage particulates. On a temporal basis, lipid normalized aliphatic concentrations peaked by the end of 2001–2002 during the rainiest period over the last four decades (1750 vs. 1083 ± 4.6 mm in 1999, 2004 and 2005), reflecting an enhanced exposition due to massive anthropogenic fluxes from Metropolitan Buenos Aires in wet years. The hydrocarbon composition in fish muscles is enriched in n-C15–17 and isoprenoids relative to a fresh crude oil and settling particulates, with fresher signatures during the 2001–2002 maxima. Fish/settling material bioaccumulation factors (BAFs: 0.4–6.4 dry weight or 0.07–0.94 lipid-organic carbon) plotted against Kow showed a parabolic pattern maximizing at n-C14–18 and isoprenoids. The optimal bioaccumulation window corresponds to highly hydrophobic (log Kow: 7.2–9.9), intermediate-size C14–18 n-alkanes and C15–20 isoprenoids (MW: 198–282; length: 17.9 to 25.4 Å) with melting points ranging from −19.8 to 28 °C. The uptake efficiency is inversely correlated to melting points and increased from 75% for n-C25 to above 90% for n-C14–15 and isoprenoids.  相似文献   

9.
A simple, rapid and sensitive GC–MS method for the determination of dithiocarbamate fungicide propineb [polymeric zinc propylenebis (dithiocarbamate)] and an improved HPLC procedure for the simultaneous determination of its main metabolite, propylenethiourea, and ethylenethiourea, the main metabolite of all ethylenedithiocarbamates, in airborne samples are described. The method for the analysis of propineb involves the evolution of carbon disulfide (CS2), under acidic conditions in the presence of stannous chloride, extraction of the generated CS2 into a layer of isooctane which is then analyzed for CS2 content by GC–MS in SIM mode. Under the optimum conditions, the retention time of CS2 was 1.89 min and the total time of chromatographic analysis was 5 min. Recoveries from spiking glass microfibre filters (GF/A) and silica gel filters were 86 ± 7 (n = 9) and 89 ± 4 (n = 9), respectively. The limit of detection is 0.7 ng per filter, which is equivalent to about 0.8–1.0 ng m−3 in air. In parallel, an HPLC method with ultraviolet detection is presented for the simultaneous analysis of the metabolites. Separation of the two metabolites was attained in less than 5 min. Recoveries from spiking GF/A and silica gel filters for ethylenethiourea were 100 ± 1 (n = 3) and 98 ± 2 (n = 3), respectively, while for propylenethiourea were 102 ± 1 (n = 3) and 98 ± 1 (n = 3), respectively. The detection limits are about 36–43 and 40–49 ng m−3 in air for ethylenethiourea and propylenethiourea, respectively. All the analytes spiked in the filters are proven to be stable for more than one month, at −4 °C.  相似文献   

10.
Shon ZH  Kim KH 《Chemosphere》2006,63(11):1859-1869
This study examines the oxidation of reduced sulfur compounds (RSCs) in urban ambient air. The photochemical conversions of RSC (such as DMS, CS2, H2S, DMDS, and CH3SH) to a further oxidized form (e.g., SO2, MSA, and H2SO4) were assessed using a photochemical box model. For our model simulation of RSC oxidation, measurements were taken at an urban monitoring station in Seoul, Korea (37.6° N, 127° E) during three separate time periods (e.g., Sept. 17–18, Oct. 23, and Oct. 27–28, 2003). The results indicate that DMS and H2S were the dominant RSCs with concentrations of 370 ± 140 and 110 ± 60 pptv, respectively. The photochemical conversion of DMDS to SO2 was found to occur more efficiently than other RSCs. The overall results of our study suggest that photochemical conversion of RSCs accounted for less than 15% of the observed SO2 during the measurement period. The SO2 production from DMS oxidation (mainly by the reaction with OH) was found to be affected primarily by the abstraction channel due to high NOx levels during the experimental conditions.  相似文献   

11.
Pyrolysis (800–900°C, ca. 5 s) of benzene/HC1 mixtures leads to chlorobenzene (1) even in a reducing environment of H2 and/or CH4. With added oxygen, 1 is formed even at 550°C; such slow combustions also yield chlorinated phenols and dibenzofurans.  相似文献   

12.
Nguyen HT  Kim KH  Kim MY  Kang CH  Shim SG 《Chemosphere》2008,71(11):2017-2029
The concentrations of total gaseous mercury (TGM) and its relevant environmental parameters were measured at a highly industrialized area in the Ban Wall industrial complex (BWIC) in An San city, Korea from March to May 2005. The mean concentrations of Hg measured during the entire study period were computed to be 6.32 ± 8.56 ng m−3 (range of 2.32–181 ng m−3; N = 1160). Due to the effects of strong man-made activities, the significantly high Hg concentration levels (e.g., at or above 10 ng m−3) comprised about 7.5% of all data with the mean of 21.8 ± 26.3 ng m−3 (N = 87). By separating the data into daytime and nighttime periods, the Hg values exhibited a notable daytime enhancement possibly due to strong man-made activities during working hours. The results of the correlation analysis indicated the possible relationship between the Hg concentration and the temperature as well as several pollutant species (e.g., NO2 and NOx). Evaluation of the Hg data in relation with the air mass transport pattern confirms that the Hg concentration levels in this industrial area are affected most eminently by local, rather than distant, pollution sources.  相似文献   

13.
Dissolved methane was monitored by means of a diffusion probe in combination with a photoacoustic (PA) detector cell placed in the cavity of a liquid nitrogen-cooled CO laser. The detection limit of the photoacoustic detector was 1 ppbv methane (≈ 2 μM in aqueous solution), the time response was 60 s, the spatial resolution was 1.36 mm. These limits were determined by the acoustic noise and the configuration of the diffusion probe. The combination of PA detector with gas diffusion probes was found to be useful for monitoring gaseous compounds. However, the membrane material of the diffusion probe was critical. Silicone as membrane material was useful only for measurement of CH4. Goretex as membrane material was applicable to measurement of dimethylsulfide (DMS), but did not give a stable signal for trimethylamine (TMA).

Vertical concentration profiles of CH4 in anoxic paddy soil agreed well with earlier results obtained with a gas chromatograph as detector. Methane was produced in anoxic soil layers below 8–10 mm depth and diffused upwards to the surface through a layer of CH4-consuming bacteria situated at about 2 mm depth. In the oxic upper 2 mm soil layer the concentration of CH4 decreased below the detection limit of our system. Methane-containing gas bubbles that were embedded in the soil were detected by a steep increase of the CH4 signal. The combination of PA detector and gas diffusion probe was found to be a useful tool to measure CH4 gradients in submerged soil or sediment with high temporal and spatial resolution, thus allowing the localization and quantification of CH4 production and CH4 oxidation rates within the soil profile.  相似文献   


14.
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   

15.
Hu Z 《Chemosphere》2008,72(2):312-318
The biokinetics of attached and suspended bacteria are an essential component of activated sludge models, anaerobic digestion models and biofilm models. These parameters are often assumed or “confirmed” based on the goodness-of-fit of the bioprocess models. Using a microbial fuel cell with a baffled reactor chamber, the attached- and mixed-growth microbial decay coefficients were evaluated under anaerobic conditions. The capability for real-time voltage recording allows easy and accurate measurement of the anaerobic microbial decay coefficients (bL, lysis-regrowth approach), which were determined to be 0.11 ± 0.01 and 0.15 ± 0.01 d−1 for attached (to anode) and mixed (present in the anode chamber) growth microorganisms, respectively. The corresponding half-saturation constants using glucose as a substrate were 204 ± 10 and 123 ± 1 mg COD l−1. Hence, like an oxygen uptake rate-based approach to measure the microbial kinetics under aerobic conditions, the electrochemical recording provides an attractive method to measure anaerobic microbial decay coefficients.  相似文献   

16.
Atmospheric Hg transfer to the forest soil through litterfall was investigated in a primary rainforest at Ilha Grande (Southeast Brazil) from January to December 1997. Litter mass deposition reached 10.0 t ha−1 y−1, with leaves composing 50–84% of the total litter mass. Concentrations of Hg in the total fallen litter varied from 20 to 244 ng g−1, with higher concentrations during the dry season, between June and August (225 ± 17 ng g−1), and lower concentrations during the rainy season (99 ± 54 ng g−1). This seasonal variability was reflected in the Hg flux through litterfall, which corresponded to a Hg input to the forest floor of 122 μg m−2 y−1, with average Hg deposition of 16.5 ± 1.5 μg m−2 month−1 during and just after the dry season (June–September) and 7.0 ± 3.6 μg m−2 month−1 in the rest of the year. The variability in meteorological conditions (determining atmospheric Hg availability to foliar scavenging) may explain the pulsed pattern of Hg deposition, since litterfall temporal variability was generally unrelated with such deposition, except by a peak in litterfall production in September. Comparisons with regional data on Hg atmospheric deposition show that litterfall promotes Hg deposition at Ilha Grande two to three orders of magnitude higher than open rainfall deposition in non-industrialized areas and approximately two times higher than open rainfall deposition in industrialized areas in Rio de Janeiro State. The observed input suggests that atmospheric Hg transfer through litterfall may explain a larger fraction of the total Hg input to forest soils in Southeast Brazil than those recorded at higher latitudes.  相似文献   

17.
Lee BN  Ying WT  Shen YT 《Chemosphere》2007,69(11):1821-1826
A modified domestic microwave oven was applied to heat a magnetite (Fe3O4) fixed-bed for continuous decomposition of volatile organic compounds (VOCs), such as acetone, n-hexane, and dichloromethane (DCM), in a simulated flue gas which contains VOCs equivalent to 2000 ppmv as DCM. Experimental results revealed that effect of the addition of water to the inlet stream on decomposition of DCM in the overall experiment was insignificant. Bulk temperature of the Fe3O4 fixed-bed was also found to reach 600 °C from an initial room temperature by 6.5 min under microwave radiation, even though the inlet gas was at a high gas hourly space velocity of 5240 h−1 and a high relative humidity of 75%. Moreover, the VOCs in the inlet stream could be decomposed completely over the Fe3O4 fixed-bed by microwave heating at a power level of 645 W at heating time of 10 min. The conversion of VOCs is stable when the Fe3O4 fixed-bed has been heated longer than 10 min with microwave radiation. The microwave-induced heating upon Fe3O4 fixed-bed processing appears to be not only an energy efficient technique for air pollutions treatment but also a promising technology for variety of VOCs in a flue gas from industrial factory being decomposed simultaneously and completely.  相似文献   

18.
A five-stage sequential leaching procedure was used to fractionate 13 heavy metals (Cd, Cu, Pb, Cr, Zn, Fe, Mn, Al, Ni, Co, As, V, Ba) and sulphur (S) in lime waste from the lime kiln at the causticizing plant of Stora Enso Oyj Veitsiluoto Pulp Mills at Kemi, Northern Finland, into the following fractions: (1) water-soluble fraction (H2O), (2) exchangeable fraction (CH3COOH), (3) easily reduced fraction (HONH3Cl), (4) oxidizable fraction (H2O2 + CH3COONH4), and (5) residual fraction (HF + HNO3 + HCl). Although metals were leachable in all fractions, the highest concentrations for most of the metals were observed in the residual fraction (stage 5). It was also notable that the total heavy metal concentrations in lime waste did not exceed the maximal allowable heavy metal concentrations for soil conditioner agents set by the ministry of the Agricultural and Forestry in Finland. The heavy metals concentrations in lime waste were also lower than the maximal allowable heavy metals concentrations of the European Union Directive 86/278/EEC on the protection of environment, and in particular of the soil, when sewage sludge is used in agriculture. The Ca concentration (420 g kg−1; d.w.) was about 262 times higher than the typical value of 1.6 g kg−1 (d.w.) in arable land in Central Finland. However, the concentration Mg (0.2 g kg−1; d.w.) in lime waste was equal to the Mg concentration in arable land in the Central Finland. The lime waste has strongly alkaline pH (12.8) and a neutralizing value (i.e. liming effect) of 47.9% expressed as Ca equivalents (d.w.). This indicates lime waste to be a potential soil conditioner and improvement as well as a pH buffer.  相似文献   

19.
Hood ED  Thomson NR  Grossi D  Farquhar GJ 《Chemosphere》2000,40(12):1383-1388
Flushing soils contaminated with trichloroethylene (TCE) and perchloroethylene (PCE) with a permanganate (MnO4) solution has been shown to reduce the solvent content of the soil. Experiments were performed to quantify the rate at which KMnO4 oxidizes aqueous solutions of PCE over a range of concentrations. In a series of homogeneous reactors, aqueous phase PCE concentrations were monitored over time in nine experimental trials with excess oxidant concentrations ranging from 5 to 30 g/l. Analysis of the data was performed to quantify the oxidation reaction order with respect to PCE and KMnO4 and the reaction rate constant. The reaction between PCE and KMnO4 was determined to be first-order with respect to both PCE and KMnO4 with an overall specific reaction rate coefficient of 2.45±0.65 M−1 min−1.  相似文献   

20.
Pikaar I  Koelmans AA  van Noort PC 《Chemosphere》2006,65(11):2343-2351
Sorption to ‘hard carbon’ (black carbon, coal, kerogen) in soils and sediments is of major importance for risk assessment of organic pollutants. We argue that activated carbon (AC) may be considered a model sorbent for hard carbon. Here, we evaluate six sorption models on a literature dataset for sorption of 12 compounds onto 12 ACs and one charcoal, at different temperatures (79 isotherms in total). A statistical analysis, accounting for differences in the number of fitting parameters, demonstrates that the dual Langmuir equation is in general superior and/or preferable to the single and triple Langmuir equation, the Freundlich equation, a Polanyi–Dubinin–Manes equation, and the Toth equation. Consequently, the analysis suggests the presence of two types of adsorption sites: a high-energy (HE) type of site and a low-energy (LE) type of site. Maximum adsorption capacities for the HE domain decreased with temperature while those for the LE domain increased. Average Gibbs free energies for adsorption from the hypothetical pure liquid state at 298 K were fairly constant at −15 ± 4 and −5 ± 4 kJ mol−1 for the HE and LE domain, respectively.  相似文献   

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