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1.
Simultaneous chloroform (CHCl3) emission and ozone (O3) deposition are regularly observed under nocturnal inversions during the summer months from and to the peat bogs in the vicinity of the Mace Head Atmospheric Research Station, Connemara, Co Galway, Ireland. Emissions were estimated using the nocturnal box model applied to routine atmospheric observations collected over a 14-year period from 1995 to 2008. Strict criteria were applied in the selection of events of low wind speed, under a stable night-time inversion layer in baseline air conditions, with no transport from Europe. The mean peatland CHCl3 flux was 2.91 μg m?2 h?1 with highly variable fluxes ranging from 0.44 to 12.94 μg m?2 h?1. These fluxes are generally larger than those reported previously for similar biomes and if representative would make a significant contribution to the global estimated source of CHCl3. Fluxes were not strongly correlated with either atmospheric temperature or the level of precipitation. Over the 14-year period there appears to have been a small increase in overall CHCl3 emissions, although we stress that the nocturnal box model has a number of limitations and assumptions which should be taken into account.  相似文献   

2.
Hourly measurements of baseline ozone at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland are observed when unpolluted air masses are advected to the station from across the North Atlantic Ocean. Monthly mean ozone mixing ratios in baseline air masses have risen steadily during the 1980s and 1990s reaching unprecedented levels during the early months of 1999. During the 2000s, baseline ozone mixing ratios have shown evidence of decline and stabilisation. Over the entire 20-year 1987–2007 period, the trend in annual baseline ozone has been +0.31±0.12(2−σ) ppb year−1 and is highly statistically significant. Trends have been highest in the spring months and lowest in the summer months, producing a significant increase in the amplitude of the seasonal cycle. Over the shorter 1995–2007 period, we demonstrate how the growth to peak in 1999 and the subsequent decline have been driven by boreal biomass burning events during 1998/1999 and 2002/2003. The 2000s have been characterised by relatively constant baseline ozone and CH4 levels and these may be a reasonable guide to future prospects, at least in the short term.  相似文献   

3.
A technique is described for identifying probable source locations for a range of greenhouse and ozone-depleting trace gases from the long-term measurements made at Mace Head, Ireland. The Met. Office's dispersion model NAME is used to predict concentrations at Mace Head from all possible sources in Europe, then source regions identified as those which consistently lead to elevated concentrations at Mace Head. Estimates of European emissions and their distribution are presented for a number of trace gases for the period 1995–1998. Estimated emission patterns are realistic, given the nature and varied applications of the species considered. The results indicate that whilst there are limitations, useful information about source distribution can be extracted from continuous measurements at a remote site. It is probable that much improved estimates could be derived if observations were available from a number of sites. The ability to assess emissions has obvious implications in monitoring compliance with internationally agreed quota and protocols.  相似文献   

4.
Two peat bogs from remote alpine sites in Australia were found to contain detailed and coherent histories of atmospheric metal pollution for Pb, Zn, Cu, Mo, Ag, As, Cd, Sb, Zn, In, Cr, Ni, Tl and V. Dramatic increases in metal deposition in the post-1850 AD portion of the cores coincide with the onset of mining in Australia. Using both Pb isotopes and metals, pollutants were ascribed to the main atmospheric pollution emitting sources in Australia, namely mining and smelting, coal combustion and agriculture. Results imply mining and metal production are the major source of atmospheric metal pollution, although coal combustion may account for up to 30% of metal pollutants. A novel finding of this study is the increase in the otherwise near-constant Y/Ho ratio after 1900 AD. We link this change to widespread and increased application of marine phosphate fertiliser in Australia's main agricultural area (the Murray Darling Basin).  相似文献   

5.
Although it occurred nearly 50 years ago, the nuclear reactor fire of October 1957 at Windscale Works, Sellafield, England, continues to attract interest. Several attempts have been made to quantify the releases of radionuclides and their radiological consequences, but additional information and a re-analysis of meteorological data encourage a further examination of emissions. The limited instrumentation of the reactor provided little relevant information and, as in previous estimates, the discharges are deduced from environmental evidence, but here the recent meteorological analysis is used. The interpretation of the meteorological and environmental evidence requires both timing and quantity of the emitted radionuclides to be considered together.Significant fission product emission continued from about 15:00 or 16:00 on 10 October 1957 until noon the following day. There were two main peaks in discharge rate, during the evening and early hours and from roughly 06:00 until 10:30, and the amounts emitted during each of these periods were probably comparable.Iodine-131 (131I), caesium-137 (137Cs) and polonium-210 (210Po) activities dominated the radioactive emissions and there is sufficient environmental evidence for releases of these radionuclides to be estimated within a factor of about two. (Some additional 131I may have escaped in a chemical form that was not included in the estimate, but it appears likely that the fraction was small.) There is evidence that the plume extended further east than accepted in previous assessments and the estimates of quantities emitted have been increased to allow for this. For other radionuclides the environmental measurements were fewer and the uncertainties are greater.  相似文献   

6.
Accurately determining methane emission factors of dairy herd in China is imperative because of China’s large population of dairy cattle. An inverse dispersion technique in conjunction with open-path lasers was used to quantify methane emissions from a dairy feedlot during the fall and winter seasons in 2009-2010. The methane emissions had a significant diurnal pattern during both periods with three emission peaks corresponding to the feeding schedule. A 10% greater emission rate in the fall season was obtained most likely by the higher methane emission from manure during that period. An annual methane emission rate of 109 ± 6.7 kg CH4 yr−1 characterized with a methane emission intensity of 32.3 ± 1.59 L CH4 L−1 of milk and a methane conversion factor (Ym) of 7.3 ± 0.38% for mature cattle was obtained, indicating the high methane emission intensity and low milk productivity in Northern China.  相似文献   

7.
Mercury (Hg) concentration profiles and historical accumulation rates were determined in three 210Pb-dated cores from a peat deposit in the vicinity of a lead (Pb) smelter at Příbram, Czech Republic. The Hg concentrations in peat samples ranged from 66 to 701 μg kg−1. Cumulative Hg inventories from each core (for the past 150 yr) varied by a factor of 1.4 (13.6–18.5 mg Hg m−2), indicating variations of net Hg accumulation rate within the peat deposit. Historical changes in vegetation cover (leading to variable interception by trees) are probably responsible for this variation in space and time. The uncorrected Hg accumulation rates peaked between the 1960s and 1980s (up to 226 μg m−2 yr−1). Recent findings show that Hg records from peat tend to overestimate historical levels of Hg deposition. Therefore we used the mass loss compensation factor (MLCF) to normalize Hg accumulation rates. These corrected Hg accumulation rates were significantly lower (maximum 129 μg m−2 yr−1) and better corresponded to changes in historical smelter emissions, which were highest in the 1960s. The agreement between the corrected Hg accumulation rates in the uppermost peat sections (2–38 μg m−2 yr−1) and biomonitoring of atmospheric deposition by mosses in several recent years (4.7–34.4 μg m−2 yr−1) shows the usefulness of MLCF application on Hg accumulation in peat archives. However, the MLCF correction was unsuitable for Pb. The recent Pb deposition rates obtained by an independent biomonitoring study using mosses (0.5–127 mg m−2 yr−1) were better correlated with net Pb accumulation rates recorded in peat (7–145 mg m−2 yr−1) than with corrected rates obtained by the MLCF approach (1–28 mg m−2 yr−1).  相似文献   

8.
A preliminary investigation has been made on the emissions of Polynuclear Aromatic Hydrocarbons (PAH) when burning wood chips and peat in a modified commercial hot water boiler. The amount of the investigated eighteen PAH that were filter trapped from peat combustion averaged 2.7 times greater than that from wood combustion per cubic meter flue gas. The total emitted amount (particulate plus gas phase PAH) was 9.7 times greater than from wood combustion. The corresponding values for benzo(a)pyrene only were 1.7 and 3.5 times greater, respectively. The comparison of PAH emitted by the combustion of wood and peat showed a pronounced tendency towards the emission of high molecular weight PAH by the latter.Particulate phase-gas phase distribution ourves are presented for PAH in the boiling point range 336°C – 525°C. In addition, the emission of a polynuclear aromatic ketone is shown.  相似文献   

9.
In this paper, methane emissions from municipal wastewater treatment plants and municipal solid waste (MSW) landfills in Jordan for 1994 have been estimated using the methodology developed by the Intergovernmental Panel on Climate Change (IPCC). For this purpose, the 14 domestic wastewater treatment plants in the country were surveyed. Generation rates and characterization of MSW components as well as dumping and landfilling practices were surveyed in order to estimate 1994 CH4 emissions from these sites. Locally available waste statistics were used in cases where those of the IPCC guidelines were not representative of Jordan's statistics. Methane emissions from domestic wastewater in Jordan were estimated at 4.66 gigagrams (Gg). Total 1994 CH4 emissions from MSW management facilities in Jordan are estimated at 371.76 Gg--351.12 Gg (94.45%) from sanitary landfills, 19.83 Gg (5.33%) from MSW open dumps, and 0.81 Gg (0.22%) from raw sewage-water dumping ponds. Uncertainties associated with these estimations are presented.  相似文献   

10.
Measurements of ammonia and particulate ammonium were made in the daytime (1200–1500) at a urban site in Yokohama during the 5-year period, 1982–1986. Diurnal NH3 concentrations showed a distinct seasonal trend with a maximum in summer. The diurnal monthly average concentrations were above 10 ppb during the late spring and summer months, while the concentrations during the winter months were between 1 and 5 ppb. The seasonal variation was found to be very similar to that of the average air temperature and showed a periodic pattern over 1 year. A good correlation was observed between diurnal NH3 concentrations and average air temperatures during the 5-year period. The annual mean concentrations were in the range of 6.6–7.6 ppb with only a minor deviation. The diurnal monthly average concentrations of particulate NH4+ were between 1 and 4 μg m−3 and no significant seasonal variations were seen. As a short-term study, simultaneous measurements of NH3, HNO3 and particulate NO3 were made. The diurnal mean concentrations of NH3 and HNO3 were 7.6 and 0.8 ppb, respectively. The concentration of particulate NO3 ranged from 0.3 to 6μg−3. Both HNO3 and particulate NO3 concentrations were relatively low and constant. Thus, NH3 and HNO3 levels did not agree with the concentrations predicted from the NH4NO3 equilibrium constant.  相似文献   

11.
The mixing ratios of HCFC-141b (1,1-dichlorofluoroethane) and HCFC-142b (1-chloro-1,1-difluoroethane) have been rising steadily in baseline air at Mace Head, Ireland over the 10-year period from 1994 to 2004. These HCFCs are widely used replacements for the chlorofluorocarbons phased out under the Montreal Protocol and its subsequent amendments. Analysis of the HCFC content of regionally-polluted air arriving at Mace Head from the European continent shows that European emissions reached a peak during 2000–2001 and have declined subsequently, following the phase-out in their usage. European emissions of HCFC-141b have been further constrained by observations at the High-Alpine Jungfraujoch site. The reductions are consistent with the phase-out of HCFC production and use from the year 2001 onwards mandated by European regulations designed to exceed the requirements of the Montreal Protocol.  相似文献   

12.
13.
Arable soils are a significant source of nitric oxide (NO), a precursor of tropospheric ozone, and thereby contribute to ozone pollution. However, their actual impact on ozone formation is strongly related to their spatial and temporal emission patterns, which warrant high-resolution estimates.Here, we combined an agro-ecosystem model and geo-referenced databases to map these sources over the 12 000 km2 administrative region surrounding Paris, France, with a kilometric level resolution. The six most frequent arable crop species were simulated, with emission rates ranging from 1.4 kg N-NO ha−1 yr−1 to 11.1 kg N-NO ha−1 yr−1. The overall emission factor for fertilizer-derived NO emissions was 1.7%, while background emissions contributed half of the total NO efflux. Emissions were strongly seasonal, being highest in spring due to fertilizer inputs. They were mostly sensitive to soil type, crops' growing season and fertilizer N rates.  相似文献   

14.
Emission of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) by municipal solid waste incinerators (MSWI) is an issue of great concern. In 1997, an adaptation to the EU legislation on pollutant emissions from the stack was carried out in an MSWI from Tarragona (Catalonia, Spain). As a result, PCDD/F emissions were significantly reduced. The aim of this study was to determine the current levels of PCDD/Fs in soil and vegetation samples collected near the facility and to compare these levels with those obtained in previous surveys (1996 and 1997). In the period 1997-1999, PCDD/F concentrations in vegetation samples were significantly decreased (60%). By contrast, the levels of PCDD/Fs in soil samples increased slightly (14%, P > 0.05) during the same period. An exhaustive analysis of the present data indicates that other emission sources of PCDD/Fs have also a notable environmental impact on the area under direct influence of the MSWI.  相似文献   

15.
16.
A method intercomparison study of analytical methods for the determination of neutral, volatile polyfluorinated alkyl substances (PFAS) was carried out in March, 2006. Environmental air samples were collected in triplicate at the European background site Mace Head on the west coast of Ireland, a site dominated by ‘clean’ westerly winds coming across the Atlantic. Extraction and analysis were performed at two laboratories active in PFAS research using their in-house methods. Airborne polyfluorinated telomer alcohols (FTOHs), fluorooctane sulfonamides and sulfonamidoethanols (FOSAs/FOSEs) as well as additional polyfluorinated compounds were investigated. Different native and isotope-labelled internal standards (IS) were applied at various steps in the analytical procedure to evaluate the different quantification strategies. Field blanks revealed no major blank problems. European background concentrations observed at Mace Head were found to be in a similar range to Arctic data reported in the literature. Due to trace-levels at the remote site, only FTOH data sets were complete and could therefore be compared between the laboratories. Additionally, FOSEs could partly be included. Data comparison revealed that despite the challenges inherent in analysis of airborne PFAS and the low concentrations, all methods applied in this study obtained similar results. However, application of isotope-labelled IS early in the analytical procedure leads to more precise results and is therefore recommended.  相似文献   

17.
Multi-year inventories of carbonaceous aerosol emissions from biomass open burning at a high spatial resolution of 0.5° × 0.5° have been constructed in China using GIS methodology for the period 1990-2005. Black carbon (BC) emissions have increased by 383.03% at an annual average rate of 25.54% from 14.05 Gg in 1990 to 67.87 Gg in 2005; while organic carbon (OC) emissions have increased by 365.43% from 57.37 Gg in 1990 to 267.00 Gg in 2005. Through the estimation period, OC/BC ratio for biomass burning was averagely 4.09, suggesting that it was not the preferred control source from a climatic perspective. Spatial distribution of BC and OC emissions were similar, mainly concentrated in three northeastern provinces, central provinces of Shandong, Jiangsu, Anhui and Henan, and southern provinces of Guangxi, Guangdong, Hunan and Sichuan basin, covering 24.89% of China’s territory, but were responsible for 63.38% and 67.55% of national BC and OC emissions, respectively.  相似文献   

18.
Studies focused on the possible use of spider webs as environmental pollution indicators. This was a first time ever attempt to use webs as indicators of polycyclic aromatic hydrocarbons (PAHs) pollution. The aim of the study was (a) to evaluate whether webs are able to accumulate PM-associated road traffic emissions and be analyzed for organic toxics such as PAHs, (b) to assess if the distance from emission sources could have an influence on the accumulation level of pollutants, and (c) to determine types of pollution sources responsible for a structure of monitoring data set. Webs of four species from the family Agelenidae were sampled for PAHs presence. Data from vehicle traffic sites (i.e., road tunnel, arterial surface road, underground parking) and from railway traffic sites (i.e., two railway viaducts) in the city of Wroclaw (Southwest of Poland) showed a significantly higher mean concentrations of PAHs than the reference site 1 (municipal water supply works). We also found a significant differences at sites differed by the distance from emission sources. The result of PCA analysis suggested three important sources of pollution. We conclude that spider webs despite of some limitations proved useful indicators of road traffic emissions; they could be even more reliable compared to use of bioindicators whose activity is often limited by a lack of water and sun.  相似文献   

19.
Asbestos fibres taken from fresh or worn brake linings or collected from the atmosphere near a freeway were examined by electron microscopy and electron diffraction. The major effect of braking appears to be in separating bunches of fibres and reducing their average length but not in altering their crystal structure. The suggestion that gross changes in the crystal structure are brought about by heat generated during braking is not supported by this work. Airborne samples were collected at points where there was considerable braking and where there was only slight braking. At the point where slight braking took place the airborne concentration was very low and could not be satisfactorily measured. At the point where considerable braking occurred an estimate of 5 × 10−5 m−3 particles was determined, each particle consisting of a small bundle of fibres. The majority of particles had a maximum linear dimension ⩽2 μn.  相似文献   

20.
Fourteen single-family detached houses in Spokane, Washington, and Coeur D'Alene, Idaho, were monitored for two years after high concentrations of indoor radon had been mitigated. Each house was monitored quarterly using mailed alpha-track radon detectors deployed in each zone of the structure. To assess performance of mitigation systems during the second heating season after mitigation, radon concentrations in seven houses were monitored continuously for several weeks, mitigation systems in all houses were inspected, and selected other measurements were taken. In addition, occupants were also interviewed regarding their maintenance, operation, and subjective evaluation of the radon mitigation systems. Quarterly alpha-track measurements showed that radon levels had increased in most of the homes during many follow-up measurement periods when compared with concentrations measured immediately after mitigation. Mitigation-system performance was adversely affected by (1) accumulated outdoor debris blocking the outlets of subsurface pressurization pipes; (2) fans being turned off (e.g., because of excessive noise or vibration); (3) air-to-air heat exchanger, basement pressurization, and subsurface ventilation fans being turned off and fan speeds reduced; and (4) crawl-space vents being closed or sealed.  相似文献   

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