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1.
ABSTRACT

Past efforts to estimate methane emissions from underground mines, surface mines, and other coal mine operations have been hampered, to different degrees, by a lack of direct emissions data. Direct measurements have been completely unavailable for several important coal mining operations. A primary goal of this study was to collect new methane emissions measurements and other data for the most poorly characterized mining operations and use these data to develop an improved methane emission inventory for the U.S. coal mining industry. This required the development and verification of measurement methods for surface mines, coal handling operations, and abandoned underground mines and the use of these methods at about 30 mining sites across the United States. Although the study's focus was on surface mines, abandoned underground mines, and coal handling operations, evaluations were also conducted to improve our understanding of underground mine emission trends and to develop improved national data sets of coal properties. Total U.S.  相似文献   

2.
This paper evaluated the feasibility of using the horizontal radial plume mapping (HRPM) technique to locate multiple emission sources via computational simulation. Seventy-two test maps, each having two Gaussian distributions, were generated in a two-dimensional domain. The HRPM technique with the non-negative least square (NNLS) algorithm was then applied to reconstruct the plumes, assuming a nine-beam scanning beam geometry. The NNLS algorithm successfully reconstructed the source locations of 68 of the 72 test maps. However, when one of the plumes was near the origin, the NNLS did not always identify the peak locations correctly. Furthermore, when the two plumes were spaced closely, the NNLS tended to reconstruct a wide plume covering both plumes instead of separating them due to the resolution limitation of the current nine-beam geometry. In the sensitivity analysis, five sets of random error (1%, 5%, 10%, 20%, and 30%) were added in the path-integrated concentration (PIC) from the 72 test maps, and thus, an additional 360 reconstructions were implemented. Robust results were obtained when the noise added was less than 20%. The results generally support the implementation of the NNLS algorithm in the HRPM technique as described in the U.S. Environmental Agency (EPA) Other Test Method 10 (OTM-10).

Implications: The methodology evaluated in this paper provides near-real-time estimates about the locations of multiple emission sources. The involved optical remote sensing instruments can monitor large spatial areas (e.g., landfills) in a cost-effective way.  相似文献   

3.
Past efforts to estimate methane emissions from underground mines, surface mines, and other coal mine operations have been hampered, to different degrees, by a lack of direct emissions data. Direct measurements have been completely unavailable for several important coal mining operations. A primary goal of this study was to collect new methane emissions measurements and other data for the most poorly characterized mining operations and use these data to develop an improved methane emission inventory for the U.S. coal mining industry. This required the development and verification of measurement methods for surface mines, coal handling operations, and abandoned underground mines and the use of these methods at about 30 mining sites across the United States. Although the study's focus was on surface mines, abandoned underground mines, and coal handling operations, evaluations were also conducted to improve our understanding of underground mine emission trends and to develop improved national data sets of coal properties. Total U.S. methane emissions are estimated to be 4.669 million tons, and as expected, emissions from underground mine ventilation and methane drainage systems dominate (74% of the total emissions). On the other hand, emissions from coal handling, abandoned underground mines, and surface mines are significant, and collectively they represent approximately 26% of the total emissions.  相似文献   

4.
On-road vehicle emission rates of nonmethane hydrocarbons (NMHCs) were measured in two tunnels in Milwaukee, WI, in summer 2000 and winter 2001. Seasonal ambient temperatures in the Midwestern United States vary more widely than in locations where most studies of NMHC emissions from vehicle fleets have been conducted. Ethanol is the added fuel oxygenate in the area, and, thus, emissions measured here are of interest as other regions phase out methyl tertiary butyl ether and increase the use of ethanol. Total emissions of NMHCs in three types of tunnel tests averaged 4560 +/- 800 mg L(-1) fuel burned (average +/- standard error). To investigate the impact of cold start on vehicle emissions, samples were collected as vehicles exited a parking structure in subzero temperatures. NMHC emissions in the subzero cold-start test were 8830 +/- 190 mg L(-1) fuel-nearly double the tunnel emissions. Comparison of ambient data for the Milwaukee area with tunnel emissions showed the impact of seasonal differences in fuels and emissions on the urban atmosphere. Composition of fuel samples collected from area gas stations in both seasons was correlated with vehicle emissions; the predominant difference was increased winter emissions of lighter hydrocarbons present in winter gasoline. A chemical mass balance model was used to determine the contributions of whole gasoline and gasoline headspace vapors to vehicle emissions in the tunnel and cold-start tests, which were found to vary with season. Results of the mass balance model also indicate that partially combusted components of gasoline are a major contributor to emissions of aromatic compounds and air toxic compounds, including benzene, toluene, xylenes, napthalene, and 1,3-butadiene, whereas air toxics hexane and 2,2,4-trimethylpentane are largely attributed to gasoline and headspace vapors.  相似文献   

5.
Electrical generation units (EGUs) are important sources of nitrogen oxides (NOx) that contribute to ozone air pollution. A dynamic management system can anticipate high ozone and dispatch EGU generation on a daily basis to attempt to avoid violations, temporarily scaling back or shutting down EGUs that most influence the high ozone while compensating for that generation elsewhere. Here we investigate the contributions of NOx from individual EGUs to high daily ozone, with the goal of informing the design of a dynamic management system. In particular, we illustrate the use of three sensitivity techniques in air quality models—brute force, decoupled direct method (DDM), and higher-order DDM—to quantify the sensitivity of high ozone to NOx emissions from 80 individual EGUs. We model two episodes with high ozone in the region around Pittsburgh, PA, on August 4 and 13, 2005, showing that the contribution of 80 EGUs to 8-hr daily maximum ozone ranges from 1 to >5 ppb at particular locations. At these locations and on the two high ozone days, shutting down power plants roughly 1.5 days before the 8-hr ozone violation causes greater ozone reductions than 1 full day before; however, the benefits of shutting down roughly 2 days before the high ozone are modest compared with 1.5 days. Using DDM, we find that six EGUs are responsible for >65% of the total EGU ozone contribution at locations of interest; in some locations, a single EGU is responsible for most of the contribution. Considering ozone sensitivities for all 80 EGUs, DDM performs well compared with a brute-force simulation with a small normalized mean bias (–0.20), while this bias is reduced when using the higher-order DDM (–0.10).

Implications: Dynamic management of electrical generation has the potential to meet daily ozone air quality standards at low cost. We show that dynamic management can be effective at reducing ozone, as EGU contributions are important and as the number of EGUs that contribute to high ozone in a given location is small (<6). For two high ozone days and seven geographic regions, EGUs would best be shut down or their production scaled back roughly 1.5 days before the forecasted exceedance. Including online sensitivity techniques in an air quality forecasting model can provide timely and useful information on which EGUs would be most beneficial to shut down or scale back temporarily.  相似文献   


6.
Crop residue burning is an extensive agricultural practice in the contiguous United States (CONUS). This analysis presents the results of a remote sensing-based study of crop residue burning emissions in the CONUS for the time period 2003-2007 for the atmospheric species of carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), nitrogen dioxide (NO2, sulfur dioxide (SO2), PM2.5 (particulate matter [PM] < or = 2.5 microm in aerodynamic diameter), and PM10 (PM < or = 10 microm in aerodynamic diameter). Cropland burned area and associated crop types were derived from Moderate Resolution Imaging Spectroradiometer (MODIS) products. Emission factors, fuel load, and combustion completeness estimates were derived from the scientific literature, governmental reports, and expert knowledge. Emissions were calculated using the bottom-up approach in which emissions are the product of burned area, fuel load, and combustion completeness for each specific crop type. On average, annual crop residue burning in the CONUS emitted 6.1 Tg of CO2, 8.9 Gg of CH4, 232.4 Gg of CO, 10.6 Gg of NO2, 4.4 Gg of SO2, 20.9 Gg of PM2.5, and 28.5 Gg of PM10. These emissions remained fairly consistent, with an average interannual variability of crop residue burning emissions of +/- 10%. The states with the highest emissions were Arkansas, California, Florida, Idaho, Texas, and Washington. Most emissions were clustered in the southeastern United States, the Great Plains, and the Pacific Northwest. Air quality and carbon emissions were concentrated in the spring, summer, and fall, with an exception because of winter harvesting of sugarcane in Florida, Louisiana, and Texas. Sugarcane, wheat, and rice residues accounted for approximately 70% of all crop residue burning and associated emissions. Estimates of CO and CH4 from agricultural waste burning by the U.S. Environmental Protection Agency were 73 and 78% higher than the CO and CH4 emission estimates from this analysis, respectively. This analysis also showed that crop residue burning emissions are a minor source of CH4 emissions (< 1%) compared with the CH4 emissions from other agricultural sources, specifically enteric fermentation, manure management, and rice cultivation.  相似文献   

7.
Assessing the public health benefits from air pollution control measures is assisted by understanding the relationship between mobile source emissions and subsequent fine particulate matter (PM2.5) exposure. Since this relationship varies by location, we characterized its magnitude and geographic distribution using the intake fraction (iF) concept. We considered emissions of primary PM2.5 as well as particle precursors SO2 and NOx from each of 3080 counties in the US. We modeled the relationship between these emissions and total US population exposure to PM2.5, making use of a source–receptor matrix developed for health risk assessment. For primary PM2.5, we found a median iF of 1.2 per million, with a range of 0.12–25. Half of the total exposure was reached by a median distance of 150 km from the county where mobile source emissions originated, though this spatial extent varied across counties from within the county borders to 1800 km away. For secondary ammonium sulfate from SO2 emissions, the median iF was 0.41 per million (range: 0.050–10), versus 0.068 per million for secondary ammonium nitrate from NOx emissions (range: 0.00092–1.3). The median distance to half of the total exposure was greater for secondary PM2.5 (450 km for sulfate, 390 km for nitrate). Regression analyses using exhaustive population predictors explained much of the variation in primary PM2.5 iF (R2=0.83) as well as secondary sulfate and nitrate iF (R2=0.74 and 0.60), with greater near-source contribution for primary than for secondary PM2.5. We conclude that long-range dispersion models with coarse geographic resolution are appropriate for risk assessments of secondary PM2.5 or primary PM2.5 emitted from mobile sources in rural areas, but that more resolved dispersion models are warranted for primary PM2.5 in urban areas due to the substantial contribution of near-source populations.  相似文献   

8.
On hot summer days in the eastern United States, electricity demand rises, mainly because of increased use of air conditioning. Power plants must provide this additional energy, emitting additional pollutants when meteorological conditions are primed for poor air quality. To evaluate the impact of summertime NOx emissions from coal-fired electricity generating units (EGUs) on surface ozone formation, we performed a series of sensitivity modeling forecast scenarios utilizing EPA 2018 version 6.0 emissions (2011 base year) and CMAQ v5.0.2. Coal-fired EGU NOx emissions were adjusted to match the lowest NOx rates observed during the ozone seasons (April 1–October 31) of 2005–2012 (Scenario A), where ozone decreased by 3–4 ppb in affected areas. When compared to the highest emissions rates during the same time period (Scenario B), ozone increased ~4–7 ppb. NOx emission rates adjusted to match the observed rates from 2011 (Scenario C) increased ozone by ~4–5 ppb. Finally in Scenario D, the impact of additional NOx reductions was determined by assuming installation of selective catalytic reduction (SCR) controls on all units lacking postcombustion controls; this decreased ozone by an additional 2–4 ppb relative to Scenario A. Following the announcement of a stricter 8-hour ozone standard, this analysis outlines a strategy that would help bring coastal areas in the mid-Atlantic region closer to attainment, and would also provide profound benefits for upwind states where most of the regional EGU NOx originates, even if additional capital investments are not made (Scenario A).

Implications: With the 8-hr maximum ozone National Ambient Air Quality Standard (NAAQS) decreasing from 75 to 70 ppb, modeling results indicate that use of postcombustion controls on coal-fired power plants in 2018 could help keep regions in attainment. By operating already existing nitrogen oxide (NOx) removal devices to their full potential, ozone could be significantly curtailed, achieving ozone reductions by up to 5 ppb in areas around the source of emission and immediately downwind. Ozone improvements are also significant (1–2 ppb) for areas affected by cross-state transport, especially Mid-Atlantic coast regions that had struggled to meet the 75 ppb standard.  相似文献   


9.
Concern regarding the impacts of continued nitrogen and sulfur deposition on ecosystem health has prompted the development of critical acid load assessments for forest soils. A critical acid load is a quantitative estimate of exposure to one or more pollutants at or above which harmful acidification-related effects on sensitive elements of the environment occur. A pollutant load in excess of a critical acid load is termed exceedance. This study combined a simple mass balance equation with national-scale databases to estimate critical acid load and exceedance for forest soils at a 1-km(2) spatial resolution across the conterminous US. This study estimated that about 15% of US forest soils are in exceedance of their critical acid load by more than 250eqha(-1)yr(-1), including much of New England and West Virginia. Very few areas of exceedance were predicted in the western US.  相似文献   

10.
Twenty-four-hour integrated gaseous NH3 and fine particulate (PM2.5)NH4+ were measured during 2004 at eight sites in the southeastern U.S. Mean NH3 concentrations for 2004 ranged from 2.44 ppbv at an urban-industrial site in North Birmingham, AL, to 0.23 ppbv at a rural-forested site near Centreville, AL. NH3 mixing ratios were found to be higher at urban sites than at nearby rural (or suburban sites) except for sites which were directly influenced by local sources. Only weak correlations with temperature were observed for NH3 at the sites; slightly greater correlations were observed for total ammonia (NHx=NH3+NH4+) vs. temperature. A weak seasonal variation was observed for NH3 mixing ratios at all sites, with all but one site exhibiting biannual maxima in spring and late summer/fall. Mean PM2.5 NH4+ concentrations ranged from 1.78μgm-3 in Atlanta, GA, to 1.02μgm-3 at Oak Grove, MS, and were more uniform across the network than NH3 mixing ratios, with only slightly larger values at urban sites as compared to nearby rural (or suburban) sites. All sites exhibited highest NHx between July and September and lowest NHx in November and December. The gaseous NH3 fraction (NH3/(NH3+NH4+)) was observed to decrease with increasing values of PM2.5 SO42- at all sites. At two rural-forested sites and two sites near the Gulf of Mexico, the NH3 gaseous fraction approached a relatively constant value of 5–10% as PM2.5SO42- increased beyond 5–7μgm-3, suggesting that NH3 availability at these locations limits aerosol neutralization.  相似文献   

11.
Air pollution control devices (APCDs) are not compulsory for medical waste incinerators (MWIs) in developing countries. In South Africa, combustion gases are usually vented directly to the atmosphere at temperatures greater than the formation temperature of dioxin. The possibility of dioxin formation outside the incinerator stack has been hypothesized. A plume model has been developed and tested in the wind tunnel with a scale model of an incinerator stack. The plume temperature and trajectory predictions of the plume model were verified within a +/- 3% experimental accuracy. Using South African data, the plume model predicts that the residence time of gases in the temperature range of 150-450 degrees C in a plume is 1.3 sec on average for 5% of a year (18 days) at meteorological conditions resulting in wind speeds of less than 1 m/sec. Two published dioxin formation models were used to assess the probability of dioxin formation in the plume. The formation models predict that the average polychlorinated dibenzodioxins/furans (PCDD/Fs) formed in the plume will exceed the stack emission regulations in South Africa of 0.2 ng/Nm3 toxic equivalent quotient (TEQ) by between 2 and 40 times. The calculated concentrations do not include additional gaseous PCDD/F compounds that may be formed at high-temperature post-combustion zones through pyrosynthesis mechanisms.  相似文献   

12.
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   

13.
Trends in fine particulate matter <2.5 microm in diameter (PM2.5) and visibility in the Southeastern United States were evaluated for sites in the Interagency Monitoring of Protected Visual Environments, Speciated Trends Network, and Southeastern Aerosol Research and Characterization Study networks. These analyses are part of the technical assessment by Visibility Improvement-State and Tribal Association of the Southeast (VISTAS), the regional planning organization for the southeastern states, in support of State Implementation Plans for the regional haze rule. At all of the VISTAS IMPROVE sites, ammonium sulfate and organic carbon (OC) are the largest and second largest contributors, respectively, to light extinction on both the 20% haziest and 20% clearest days. Ammonium nitrate, elemental carbon (EC), soils, and coarse particles make comparatively small contributions to PM2.5 mass and light extinction on most days at the Class I areas. At Southern Appalachian sites, the 20% haziest days occur primarily in the late spring to fall, whereas at coastal sites, the 20% haziest days can occur through out the year. Levels of ammonium sulfate in Class I areas are similar to those in nearby urban areas and are generally higher at the interior sites than the coastal sites. Concentrations of OC, ammonium nitrate, and, sometimes, EC, tend to be higher in the urban areas than in nearby Class I areas, although differences in measurement methods complicate comparisons between networks. Results support regional controls of sulfur dioxide for both regional haze and PM2.5 implementation and suggest that controls of local sources of OC, EC, or nitrogen oxides might also be considered for urban areas that are not attaining the annual National Ambient Air Quality Standard for PM2.5.  相似文献   

14.
In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NOx) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NOx emissions reductions imposed on the utility sector by the NOx State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NOx emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NOx SIP Call. Comparison of the "no-control" with the "2002" scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NOx emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.  相似文献   

15.
A regional modeling system was applied with inputs from global climate and chemistry models to quantify the effects of global change on future biogenic emissions and their impacts on ozone and biogenic secondary organic aerosols (BSOA) in the US. Biogenic emissions in the future are influenced by projected changes in global and regional climates and by variations in future land use and land cover (LULC). The modeling system was applied for five summer months for the present-day case (1990–1999, Case 1) and three future cases covering 2045–2054. Individual future cases were: present-day LULC (Case 2); projected-future LULC (Case 3); and future LULC with designated regions of tree planting for carbon sequestration (Case 4). Results showed changing future meteorology with present-day LULC (Case 2) increased average isoprene and monoterpene emission rates by 26% and 20% due to higher temperature and solar insolation. However when LULC was changed together with climate (Case 3), predicted isoprene and monoterpene emissions decreased by 52% and 31%, respectively, due primarily to projected cropland expansion. The reduction was less, at 31% and 14% respectively, when future LULC changes were accompanied by regions of tree planting (Case 4). Despite the large decrease in biogenic emission, future average daily maximum 8-h (DM8H) ozone was found to increase between +8 ppbv and +10 ppbv due to high future anthropogenic emissions and global chemistry conditions. Among the future cases, changing LULC resulted in spatially varying future ozone differences of ?5 ppbv to +5 ppbv when compared with present-day case. Future BSOA changed directly with the estimated monoterpene emissions. BSOA increased by 8% with current LULC (Case 2) but decreased by 45%–28% due to future LULC changes. Overall, the results demonstrated that on a regional basis, changes in LULC can offset temperature driven increases in biogenic emissions, and, thus, LULC projection is an important factor to consider in the study of future regional air quality.  相似文献   

16.
Analyses of U.S. Environmental Protection Agency (EPA) certification data, California Air Resources Board surveillance testing data, and EPA research testing data indicated that EPA's MOBILE6.2 emission factor model substantially underestimates emissions of gaseous air toxics occurring during vehicle starts at cold temperatures for light-duty vehicles and trucks meeting EPA Tier 1 and later standards. An unofficial version of the MOBILE6.2 model was created to account for these underestimates. When this unofficial version of the model was used to project emissions into the future, emissions increased by almost 100% by calendar year 2030, and estimated modeled ambient air toxics concentrations increased by 6-84%, depending on the pollutant. To address these elevated emissions, EPA recently finalized standards requiring reductions of emissions when engines start at cold temperatures.  相似文献   

17.
This is the consolidated report of emissions of PCDD/F from facilities in the organic chemical manufacturing chain leading to polyvinyl chloride. Data have been gathered from facilities in the US and Canada from a number of manufacturers and at various steps in the manufacturing process. Estimates of US emissions or transfers of PCDD/F were generated on an "Upper Bound" and "Most Likely" basis. The Most Likely estimate of US emissions of PCDD/F to the open environment, that is, air, water and land surface by facilities in this chain, based on evaluation of non-detects at one-half the detection limit is about 12 g I-TEQ per year. On this same basis, an estimated 19 g is disposed of in secure landfills.  相似文献   

18.
Ferrario J  Byrne C  Schaum J 《Chemosphere》2007,67(9):1816-1821
Processed ball clays commonly used by the ceramic art industry in the United States were collected from retail suppliers and analyzed for the presence and concentration of the 2,3,7,8-Cl substituted polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/PCDFs). The average PCDD toxic equivalent (TEQ) concentrations of these processed ball clays was approximately 800 pg/g (TEQ-WHO) with characteristic congener profiles and isomer distributions similar to patterns of previously analyzed raw and processed ball clays. The PCDF concentrations were below the average limit of detection (LOD) of 0.5 pg/g. Correlation analyses reveal no significant relationship between total organic carbon (TOC) and either individual, homologues, and total tetra-through octa-chlorinated PCDD congeners, or TEQ concentrations of the processed ball clays. The results are consistent with earlier studies on levels of PCDDs in ball clays. Data from earlier studies indicated that dioxins may be released to the environment during the processing of raw clay or the firing process used in commercial ceramic facilities. The presence of dioxin in the clays also raises concerns about potential occupational exposure for individuals involved in the mining/processing of ball clay, ceramics manufacturing and ceramic artwork.  相似文献   

19.
Evaluating the air pollution impacts of energy use in the industrial sector is difficult because of the diversity and multiplicity of sources and a general lack of systematic, up-to-date data collection mechanisms. Fuel-specific energy consumption for a multi-state region is provided by the U.S. Department of Energy PIES model for a base year (1975), together with scenarios for future years. A computer model developed in this study—the Sub-regional Energy and Emissions Model (SEEM)—is applied to disaggregate the regional industrial figures to the county level according to fuel type and industrial category at the two-digit SIC level. The resulting emissions of total suspended particulates (TSP) and sulfur dioxide (SO2) for all industrial categories are estimated at the county level by Incorporating county-specific air pollution regulations in SEEM, and are then aggregated to larger geographical regions. The model has been applied to evaluate the increased air pollution impacts of industrial energy use in the northeastern United States for two alternative 1990 scenarios: (1) the midrange/trendlong PIES projections, and (2) a Coal Replacement Scenario, which assumes a higher percentage of fuel burned in new boilers will be coal. The results are discussed in terms of implications for air pollution control policy.  相似文献   

20.
Methane emissions from the peat bogs in Connemara, Ireland have been inferred from the trace gas observations at the Mace Head Atmospheric Research Station using the nocturnal box method. A total of 237 local events, during April to September, over a 12-year period have been studied. Simultaneous emissions of methane, carbon dioxide and chloroform are routinely observed under nocturnal inversions with low wind speeds from the peat bogs proximal to Mace Head. Night-time deposition of ozone and hydrogen occurs concurrently with these emissions. Using the temporally correlated methane and ozone data we estimate methane emissions from each event. Simultaneous methane and chloroform emissions, together with ozone and hydrogen deposition have been characterised, leading to the estimation of methane emission rates for each event. The mean methane emission flux was found to be 400 ± 90 ng m?2 s?1. A strong seasonal cycle was found in the methane emission fluxes but there was little evidence of a long-term trend in the emissions from the peat bogs in the vicinity of the Mace Head station.  相似文献   

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