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1.
Measurements of carbon dioxide (CO2) concentration were made at a coastal land station, Goa, on the west coast of India from March to June 2003 as part of the ARMEX (ARabian sea Monsoon Experiment) campaign. The observations show a systematic reduction (~120?mg?m?3) of CO2 concentration during the pre-monsoon months, March–May, during which no significant change in anthropogenic emissions takes place. CO2 shoots up from 520 to 635?mg?m?3 in June with the onset of the South West monsoon. Back trajectories show that the source of air mass gradually shifts from the coastal land mass to the open southern Arabian Sea during the pre-monsoon period. The observed reduction in CO2 is explained in terms of earlier measurements in the Arabian Sea indicating maximum chlorophyll a (Sarupria and Bhargava in J Mar Sci 27:292–297, 1998) and minimum partial pressure of CO2 (Sarma in J Geophys Res 108:3225, 2003) in the sea waters off the west coast of India during the pre-monsoon period, cleaner marine air mass advection from the open sea, and negligible local vertical CO2 flux.  相似文献   

2.
A meteorological analysis is presented for environmental data set obtained from the Canadian Arctic haze study, which is part of AGASP-II. Results of the study indicated that atmospheric carbon dioxide (CO2), methane (CH4), sulphate (SO4 =), ozone (O3) and other air pollutants observed at Alert, N.W.T. underwent periodical fluctuations. It was found that high concentrations of these atmospheric constituents were associated with a deep (1430–2074 m) inversion and with a major anticyclone. In contrast, relatively low values of these constituents were associated with a cyclonic disturbance near Alert. High concentrations of these constituents occurred with air trajectories coming from the N-W direction, while low values occurred with S trajectories. In addition, examinations of satellite imagery with other meteorological data suggested that volcanic inputs of ash and gases from Augustine Island, Alaska were negligible for the observed high values of these constituents at the ground level at Alert.  相似文献   

3.
Fifty flask air samples were taken during April 1986 from a NOAA WP-3D Orion aircraft which flew missions across a broad region of the Arctic as part of the second Arctic Gas and Aerosol Sampling Program (AGASP II). The samples were subsequently analyzed for both carbon dioxide (CO2) and methane (CH4). The samples were taken in well-defined layers of Arctic haze, in the background troposphere where no haze was detected, and from near the surface to the lower stratosphere. Vertical profiles were specifically measured in the vicinity of Barrow, Alaska to enable comparisons with routine surface measurements made at the NOAA/GMCC observatory. Elevated levels of both methane and carbon dioxide were found in haze layers. For samples taken in the background troposphere we found negative vertical gradients (lower concentrations aloft) for both gases. For the entire data set (including samples collected in the haze layers) we found a strong positive correlation between the methane and carbon dioxide concentrations, with a linear regression slope of 17.5 ppb CH4/ppm CO2, a standard error of 0.6, and a correlation coefficient (r2) of 0.95. This correlation between the two gases seen in the aircraft samples was corroborated by in situ surface measurements of these gases made at the Barrow observatory during March and April 1986. We also find a similar relationship between methane and carbon dioxide measured concurrenty for a short period in the moderately polluted urban atmosphere of Boulder, Colorado. We suggest that the strong correlation between methane and carbon dioxide concentrations reflects a common source region for both, with subsequent long-range transport of the polluted air to the Arctic.  相似文献   

4.
Abstract

Arctic haze has been attributed to industrial pollution released at mid‐latitudes. Our current understanding has been pieced together from routine meteorological data, ground‐based air chemistry observations and limited aircraft measurements. This study investigates the relationship between synoptic boundary‐layer meteorology and the composition of the near‐surface atmosphere during the polar sunrise at Alert, N.W.T. A secondary objective is to characterize the influence of local activity on the atmospheric composition at a site for a new baseline monitoring station and at a location where aerosol chemistry and grab‐flask samples for CO2 have been made for many years. Detailed measurements of the vertical distribution of aerosols were obtained from an upward‐looking lidar to complement the ground‐based measurements. Meteorological profiles of the near‐surface boundary layer were obtained from both free‐flying and tethered balloons. Near‐surface measurements were made of aerosol physical and chemical properties, O3, NO2, NO/NOx, Peroxyacetylnitrate (PAN) and hydrocarbons.

The study period was characterized by prolonged periods with strong surface inversions, which were broken up occasionally by intrusions of cold air into the warmer air aloft. Lidar observations showed that ice crystals often accompanied aerosols and were responsible for reducing visibility below 30–40 km. There was a strong correlation between aerosol mass in the diameter size range 0.15 to 1.5 μm and total SO4 = . PAN found at concentrations of about 200 ppt(v) was the main carrier of atmospheric nitrogen. Aerosol trace elements were divisible into anthropogenic soil, mixed soil/anthropogenic sea salt and halogens. Vertical transport in the surface boundary layer, as regulated by the strength of the surface radiation inversion, may play an important role in influencing the chemical composition of the air at the ground. The location of the new baseline monitoring laboratory was found to be generally windier and warmer than the lower altitude weather station, and the influence of local activity was found to be minimal.  相似文献   

5.
As part of the second Arctic Gas and Aerosol Sampling Program (AGASP II) continuous measurements of atmospheric aerosol black carbon (BC) were made at the NOAA/GMCC observatory at Barrow, Alaska (71°19N, 156°36W) during the period March 21–April 22, 1986. Black carbon is produced only by incomplete combustion of carbonaceous materials and so is a particularly useful atmospheric indicator of anthropogenic activities. The BC data have been analyzed together with the concurrent measurements of carbon dioxide (CO2), methane (CH4), and condensation nuclei (CN) that are routinely made at the observatory. All four species showed elevated and highly variable concentrations due to local human activities, principally in the township of Barrow, 7 km to the southwest, and at the DEW Line radar installation 1 km to the northwest. We distinguish between those periods of the record that are affected by local activities and those that are not, on the basis of the short-term (periods of up to 1 hour) variability of the continuous CO2 and CN records, with large short-term variabilities indicating local sources. We identified seven periods of time (events) with durations ranging from 13 to 37 hours when the BC, CO2, and CH4 concentrations changed smoothly over time, were highly correlated with each other, and were not influenced by local activities. These events had BC/CO2 ratios in the range (50–103)×10–6. These ratios are dimensionless since we convert the CO2 concentrations to units of ng m–3 of carbon. Such values of BC/CO2 are characteristic of the combustion effluent from large installations burning heavy fuel oil or coal, automobiles, and domestic-scale natural gas usage. We conclude that these events are indicative of air masses that have been polluted with combustion emissions in a distant location and then transported to the Arctic. In the absence of species-selective loss mechanisms, these air masses will maintain their combustion effluent signatures during the transport. The BC/CO2 ratios found for the local combustion activities are consistent with those expected from known combustion processes.  相似文献   

6.
Six years of observations (1980 to 1986) of the composition of lower tropospheric aerosols at Alert on northern Ellesmere Island in the Canadian high Arctic yield insight into the seasonal variation of Arctic air pollutants as well as of substances of natural origin. A principal component analysis of 138 observations of 21 aerosol constituents (major ions, metals, nonmetallic trace elements) for the most polluted period of December to April identified not only a soil, sea salt and anthropogenic aerosol component, but also one associated with photochemical reactions in the atmosphere that occur at polar sunrise. Depending on the source of their gaseous precursors, elements in the photochemical component can be natural or anthropogenic in origin. For instance, SO4 2-, existing mostly as H2SO4, originates probably from both anthropogenic and natural sources while Br– is likely of marine origin. In contrast, SO4 2- in the anthropogenic component has the stoichiometry of NH4HSO4. In the winter months, over 90% of Arctic SO4 2- is in the anthropogenic and photochemical components.In winter, a substantial portion (11 to 35%) of Na+ is associated with the anthropogenic aerosol component suggesting either that marine aerosols have been physically or chemically modified by interactions with air pollution or that there are anthropogenic sources of Na+.The aerosol soil component is controlled by both local and distant dust sources. During a year, it has two peaks at Alert, one in April/May coinciding with the Asian dust storm season and one in September.There is a marked difference in the seasonal variation of particulate Br– and iodine concentrations in the air. Both have a peak in April/May associated with polar sunrise and, hence, photochemical reactions in the atmosphere. However, iodine also peaks in early fall. This may be a product of biogenic iodine emissions to the atmosphere during secondary blooms in northern oceans in late summer.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988  相似文献   

7.
Measurements of carbon dioxide(CO2), methane(CH4), and carbon monoxide(CO) are of great importance in the Qinghai-Tibetan region, as it is the highest and largest plateau in the world affecting global weather and climate systems. In this study, for the first time, we present CO2, CH4, and CO column measurements carried out by a Bruker EM27/SUN Fourier-transform infrared spectrometer(FTIR) at Golmud(36.42°E, 94.91°N, 2808 m) in August 2021. The mean and...  相似文献   

8.
Emissions of N2O, CH4, and CO2 from soils at two sites in the tropical savanna of central Venezuela were determined during the dry season in February 1987. Measured arithmetic mean fluxes of N2O, CH4, and CO2 from undisturbed soil plots to the atmosphere were 2.5×109, 4.3×1010, and 3.0×1013 molecules cm-2 s-1, respectively. These fluxes were not significantly affected by burning the grass layer. Emissions of N2O increased fourfold after simulated rainfall, suggesting that production of N2O in savanna soils during the rainy season may be an important source for atmospheric N2O. The CH4 flux measurements indicate that these savanna soils were not a sink, but a small source, for atmospheric methane. Fluxes of CO2 from savanna soils increased ninefold two hours after simulated rainfall, and remained three times higher than normal after 16 hours. More research is needed to clarify the significance of savannas in the global cycles of N2O, CH4, CO2, and other trace gases, especially during the rainy season.  相似文献   

9.
In this paper we quantify the CH4, CO2 and NO x emissions during routine operations at a major oil and gas production facility, Prudhoe Bay, Alaska, using the concentrations of combustion by products measured at the NOAA-CMDL observatory at Barrow, Alaska and fuel consumption data from Prudhoe Bay. During the 1989 and 1990 measurement campaigns, 10 periods (called events) were unambiguously identified where surface winds carry the Prudhoe Bay emissions to Barrow (approximately 300 km). The events ranged in duration from 8–48 h and bring ambient air masses containing substantially elevated concentrations of CH4, CO2 and NO y to Barrow. Using the slope of the observed CH4 vs CO2 concentrations during the events and the CO2 emissions based on reported fuel consumption data, we calculate annual CH4 emissions of (24+/–8)×103 metric tons from the facility. In a similar manner, the annual NO x emissions are calculated to be (12+/–4)×103 metric tons, which is in agreement with an independently determined value. The calculated CH4 emissions represent the amount released during routine operations including leakage. However this quantity would not include CH4 released during non-routine operations, such as from venting or gas flaring.  相似文献   

10.
There are large uncertainties in identifying and quantifying the natural and anthropogenic sources of chloromethanes – methyl chloride (CH3Cl), chloroform (CHCl3) and dichloromethane (CH2Cl2), which are responsible for about 15% of the total chlorine in the stratosphere. We report two years of in situ observations of these species from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41° S, 145° E). The average background levels of CH3Cl, CHCl3 and CH2Cl2 during 1998–2000 were 551± 8, 6.3± 0.2 and 8.9± 0.2 ppt (dry air mole fractions expressed in parts per 1012) respectively, with a two-year average amplitude of the seasonal cycles in background air of 25, 1.1 and 1.5 ppt respectively. The CH3Cl and CHCl3 records at Cape Grim show clear episodes of elevated mixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated, suggesting common source(s). Trajectory analyses show that the sources of CH3Cl and CHCl3 that are responsible for these elevated observations are located in coastal-terrestrial and/or coastal-seawater regions in Tasmania and the south-eastern Australian mainland. Elevated levels of CH2Cl2 (up to 70 ppt above background) are associated mainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim.Now at the Centre for Atmospheric ChemistryNow at School of Environmental Sciences  相似文献   

11.
Greenhouse Gas Emissions from Hydroelectric Reservoirs in Tropical Regions   总被引：2，自引：1，他引：2  
This paper discusses emissions by power-dams in the tropics. Greenhouse gas emissions from tropical power-dams are produced underwater through biomass decomposition by bacteria. The gases produced in these dams are mainly nitrogen, carbon dioxide and methane. A methodology was established for measuring greenhouse gases emitted by various power-dams in Brazil. Experimental measurements of gas emissions by dams were made to determine accurately their emissions of methane (CH4) and carbon dioxide (CO2) gases through bubbles formed on the lake bottom by decomposing organic matter, as well as rising up the lake gradient by molecular diffusion.The main source of gas in power-dams reservoirs is the bacterial decomposition (aerobic and anaerobic) of autochthonous and allochthonous organic matter that basically produces CO2 and CH4. The types and modes of gas production and release in the tropics are reviewed.  相似文献   

12.
Anthropogenic emissions of methane (CH4) and nitrous oxide (N2O) from livestock agriculture (enteric fermentation, animal waste management systems, and pasture manure) and plant growing of the Russia (CH4 emissions from rice fields, direct and indirect N2O emissions from agricultural lands) are considered. In 2004, the total emissions of these greenhouse gases in the agricultural sector amounted to 1.4 × 105 thousand t CO2-equivalent, which corresponds to 45% of the 1990 level (3.1 × 105 thousand t CO2-equivalent). In 2004, the contribution of N2O to the total agricultural emissions was approximately twice (67.0%) that of CH4 (33.0%). Direct N2O emissions from agricultural soils (0.5 × 105 thousand t CO2-equivalent) and CH4 emissions from the internal fermentation of domestic animals (0.4 × 105 thousand t CO2-equivalent) are the most significant sources in the agricultural sector of the Russian Federation. In 2004, all these agricultural sources emitting methane and nitrous oxide contributed about 7% CO2-equivalent to the total emission of the anthropogenic greenhouse gases in Russia.  相似文献   

13.
Very few studies have conducted long-term observations of methane (CH4) flux over forest canopies. In this study, we continuously measured CH4 fluxes over an evergreen coniferous (Japanese cypress) forest canopy throughout 1?year, using a micrometeorological relaxed eddy accumulation (REA) system with tuneable diode laser spectroscopy (TDLS) detection. The Japanese cypress forest, which is a common forest type in warm-temperate Asian monsoon regions with a wet summer, switched seasonally between a sink and source of CH4 probably because of competition by methanogens and methanotrophs, which are both influenced by soil conditions (e.g., soil temperature and soil moisture). At hourly to daily timescales, the CH4 fluxes were sensitive to rainfall, probably because CH4 emission increased and/or absorption decreased during and after rainfall. The observed canopy-scale fluxes showed complex behaviours beyond those expected from previous plot-scale measurements and the CH4 fluxes changed from sink to source and vice versa.  相似文献   

14.
Methyl Chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion (Carpenter et al. 2014). In the global CH3Cl budget, the atmospheric CH3Cl emissions is predominantly maintained by natural sources, of which magnitudes have been relatively well-constrained. However, significant uncertainties still remain in the CH3Cl emission strengths from anthropogenic sources. High-frequency and high-precision in situ measurements of atmospheric CH3Cl concentrations obtained since 2008 at Gosan station (a remote background site in the East Asia) reveal significant pollution events superimposed on the seasonally varying regional background levels. Back trajectory statistics showed that air masses corresponding to the observed CH3Cl enhancement largely originated from regions of intensive industrial activities in China. Based on an inter-species correlation method, estimates of CH3Cl emissions from manufacturing industries including coal combustion, use of feedstocks, or process agents in chemical production for China (2008–2012) are 297 ± 71 Gg yr.?1 in 2008 to 480 ± 99 Gg yr.?1 in 2009, followed by a gradual decrease of about 25% between 2009 and 2012 (398 ± 92 Gg yr.?1 for 2010; 286 ± 68 Gg yr.?1 for 2011; 358 ± 92 Gg yr.?1 for 2012). The annual average of industrial CH3Cl emissions for 2008–2012 (363 ± 85 Gg yr.?1) in China is comparable to the known total global anthropogenic CH3Cl emissions accounting only for coal combustion and indoor biofuel use. This may suggest that unless emissions from the chemical industry are accounted for, global anthropogenic emissions of CH3Cl have been substantially underestimated. In particular, since industrial production and use of CH3Cl have not been regulated under the Montreal Protocol (MP) or its successor amendments, continuous monitoring of Chinese CH3Cl outflow is important to properly evaluate its anthropogenic emissions.  相似文献   

15.
Presented is the assessment of the contribution that such major types of the land use in Russia as arable lands, forage lands, settlements, and peatery make to anthropogenic fluxes of carbon dioxide CO2, methane CH4, and nitrogen oxide N2O, The assessment is based on the methods of computation monitoring carried out in the period from 2000 to 2011. The results of the study demonstrated that every year arable lands cause the emission of CO2 and N2O of about 117.0 and 74.9 million t CO2 equiv, and peatery, 0.54 and 105.4 thousand t CO2 equiv, respectively. The balance of soil carbon in hayfields and pastures is close to zero. The average emissions of CH4 and N2O from the manure of pasture animals amount to 0.2 and 5.0 million t CO2 equiv/year, and those from grass fires, 276.1 and 372.5 thousand t CO2 equiv/year, respectively. The carbon balance in permanent soils of settlements is also almost close to zero, and newly built-up lands are the source of CO2 (9.5 million t/year). The natural overgrowing of fallow lands leads to the accumulation of the soil carbon (about 92.4 million t CO2/year). It was revealed that the intensity of CO2 emission is defined by the soil carbon balance and that of other gases, by the amount of nitrogen fertilizers, plant residues, and manure coming to the soil. The total emission from the land use is 106.9 million t CO2 equiv/year that makes up 4.9% of the total anthropogenic emission of greenhouse gases in the Russian Federation.  相似文献   

16.
Aerosols consist of organic and inorganic species, and the composition and concentration of these species depends on their sources, chemical transformation and sinks. In this study an assessment of major inorganic ions determined in three aerosol particle size ranges collected for 1 year at Welgegund in South Africa was conducted. SO42? and ammonium (NH4+) dominated the PM1 size fraction, while SO42? and nitrate (NO3) dominated the PM1–2.5 and PM2.5–10 size fractions. SO42? had the highest contribution in the two smaller size fractions, while NO3? had the highest contribution in the PM2.5–10 size fraction. SO42? and NO3? levels were attributed to the impacts of aged air masses passing over major anthropogenic source regions. Comparison of inorganic ion concentrations to levels thereof within a source region influencing Welgegund, indicated higher levels of most species within the source region. However, the comparative ratio of SO42? was significantly lower due to SO42? being formed distant from SO2 emissions and submicron SO42? having longer atmospheric residencies. The PM at Welgegund was determined to be acidic, mainly due to high concentrations of SO42?. PM1 and PM1–2.5 fractions revealed a seasonal pattern, with higher inorganic ion concentrations measured from May to September. Higher concentrations were attributed to decreased wet removal, more pronounced inversion layers trapping pollutants, and increases in household combustion and wild fires during winter. Back trajectory analysis also revealed higher concentrations of inorganic ionic species corresponding to air mass movements over anthropogenic source regions.  相似文献   

17.
Carbon dioxide, methane, and carbon monoxide are the carbon cycle gases, the data on their emissions are needed when monitoring air pollution and developing methods for reducing anthropogenic emissions to the atmosphere and for climate forecasting. The estimates of nocturnal area fluxes for CO2, CH4, and CO presented for a suburb of Saint Petersburg (Peterhof) are obtained using the box model and continuous observations of concentration of these gases. The mean values of CH4, CO2, and CO fluxes estimated for Peterhof for 2014–2015 are 44 ± 27, 6100 ± 4000, and 90 ± 100 t/(km2 year), respectively. The intensity of the CO area flux has pronounced seasonal variations characterized by the maximum of ~(160 ± 120) t/(km2 year) in November—February and by the minimum of ~(30 ± 20) t/(km2 year) in June-July. The analysis of the ratio of CO/CO2 fluxes identified the main types of anthropogenic sources typical of Peterhof: motor transport, natural gas combustion, and the use of wood stoves for the heating of private low-rise buildings (in the cold season).  相似文献   

18.
Developed regions of the world represent a major atmospheric methane(CH_4) source, but these regional emissions remain poorly constrained. The Yangtze River Delta(YRD) region of China is densely populated(about 16% of China's total population) and consists of large anthropogenic and natural CH_4 sources. Here, atmospheric CH_4 concentrations measured at a 70-m tall tower in the YRD are combined with a scale factor Bayesian inverse(SFBI) modeling approach to constrain seasonal variations in CH_4 emissions. Results indicate that in 2018 agricultural soils(AGS, rice production) were the main driver of seasonal variability in atmospheric CH_4 concentration. There was an underestimation of emissions from AGS in the a priori inventories(EDGAR—Emissions Database for Global Atmospheric Research v432 or v50), especially during the growing seasons. Posteriori CH_4 emissions from AGS accounted for 39%(4.58 Tg, EDGAR v432) to 47%(5.21 Tg, EDGAR v50) of the total CH_4 emissions. The posteriori natural emissions(including wetlands and water bodies) were1.21 Tg and 1.06 Tg, accounting for 10.1%(EDGAR v432) and 9.5%(EDGAR v50) of total emissions in the YRD in2018. Results show that the dominant factor for seasonal variations in atmospheric concentration in the YRD was AGS,followed by natural sources. In summer, AGS contributed 42%(EDGAR v432) to 64%(EDGAR v50) of the CH_4 concentration enhancement while natural sources only contributed about 10%(EDGAR v50) to 15%(EDGAR v432). In addition, the newer version of the EDGAR product(EDGAR v50) provided more reasonable seasonal distribution of CH_4 emissions from rice cultivation than the old version(EDGAR v432).  相似文献   

19.
China’s first carbon dioxide(CO2) measurement satellite mission, TanSat, was launched in December 2016. This paper introduces the first attempt to detect anthropogenic CO2 emission signatures using CO2 observations from TanSat and NO2 measurements from the TROPOspheric Monitoring Instrument(TROPOMI) onboard the Copernicus Sentinel-5 Precursor(S5P) satellite. We focus our analysis on two selected cases in Tangshan, China and Tokyo, Japan.We found that t...  相似文献   

20.
There are large uncertainties in identifying and quantifying the globally significant sources and sinks of methyl bromide (CH3Br) and methyl iodide (CH3I). Long-term, quasi-continuous observations can provide valuable information about their regional sources, which may be significant in the global context. We report 3 years of in situobservations of these trace gases from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41 °S, 145 °E). The average background levels of CH3Br and CH3I during March 1998–March 2001 were 8.05 and 1.39 ppt (dry air mole fractions expressed in parts per 1012), respectively. The CH3Br background data showed little seasonal variability. Trajectory analyses reveal that air masses showing elevated CH3Br levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater and/or urban source regions. The CH3I background data showed a seasonal cycle with a 3-year average amplitude of 0.47 ppt and maximum concentrations in summer, suggesting that the Southern Ocean is a significant source.Trajectory analyses reveal that air masses showing highly elevated CH3I levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater regions and/or the open-ocean regions of Bass Strait and the Tasman Sea.  相似文献   

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