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1.
Partially speciated hydrocarbon (HC) emissions data from several small utility engines, as measured by a Fourier Transform Infrared analyzer, are presented. The engines considered have nominal horsepower ratings between 3.7 and 9.3 kW. Both side-valve and overhead-valve engines are studied, and four different fuels are used in the engines. The results indicate that the small HCs present in the exhaust tend to be in the form of either methane or unsaturated HCs. Other small alkanes, such as ethane and propane, are present in only relatively small concentrations. In terms of ozone formation potential, the HCs in the form of methane will lead to little ozone, but the distribution of the C2 and C3 species is not ideal from an ozone reduction stand-point. It is also found that the presence of oxygen in the fuels appears to lead to somewhat more complete combustion, although the effects are not large. Finally, the overhead-valve engines appear to have lower HC emissions than side-valve engines, which is primarily due to higher operating A/F ratios and the engine geometry.  相似文献   

2.
The present paper presents results from the analysis of 29 individual C2–C9 hydrocarbons (HCs) specified in the European Commission Ozone Directive. The 29 HCs are measured in exhaust from common, contemporary vehicle/engine/fuel technologies for which very little or no data is available in the literature. The obtained HC emission fingerprints are compared with fingerprints deriving from technologies that are being phased out in Europe. Based on the total of 138 emission tests, thirteen type-specific fingerprints are extracted (Mean ± SD percentage contributions from individual HCs to the total mass of the 29 HCs), essential for receptor modelling source apportionment. The different types represent exhaust from Euro3 and Euro4 light-duty (LD) diesel and petrol-vehicles, Euro3 heavy-duty (HD) diesel exhaust, and exhaust from 2-stroke preEuro, Euro1 and Euro2 mopeds. The fuels comprise liquefied petroleum gas, petrol/ethanol blends (0–85% ethanol), and mineral diesel in various blends (0–100%) with fatty acid methyl esters, rapeseed methyl esters palm oil methyl esters, soybean oil methyl or sunflower oil methyl esters. Type-specific tracer compounds (markers) are identified for the various vehicle/engine/fuel technologies.An important finding is an insignificant effect on the HC fingerprints of varying the test driving cycle, indicating that combining HC fingerprints from different emission studies for receptor modelling purposes would be a robust approach.The obtained results are discussed in the context of atmospheric ozone formation and health implications from emissions (mg km?1 for LD and mopeds and mg kW h?1 for HD, all normalised to fuel consumption: mg dm?3 fuel) of the harmful HCs, benzene and 1,3-butadiene.Another important finding is a strong linear correlation of the regulated “total” hydrocarbon emissions (tot-HC) with the ozone formation potential of the 29 HCs (ΣPO3 = (1.66 ± 0.04) × tot-RH; r2 = 0.93). Tot-HC is routinely monitored in emission control laboratories, whereas C2–C9 are not. The revealed strong correlations broadens the usability of data from vehicle emission control laboratories and facilitates the comparison of the ozone formation potential of HCs in exhaust from of old and new vehicle/engine/fuel technologies.  相似文献   

3.
The objective of this study was to characterize exhaust emissions from a series of handheld, 2-stroke small engines. A total of 23 new and used engines from model years 1981–2003 were studied; these engines spanned three phases of emission control (pre-control, phase-1, phase-2). Measured emissions included carbon monoxide (CO), carbon dioxide (CO2), nitrogen oxides (NOx), hydrocarbons (HC), fine particulate matter (PM2.5), and sulfur dioxide (SO2). Emissions reductions in CO (78%) and HC (52%) were significant between pre-control and phase-2 engines. These reductions can be attributed to improvements in engine design, reduced scavenging losses, and implementation of catalytic exhaust control. Total hydrocarbon emissions were strongly correlated with fuel consumption rates, indicating varying degrees of scavenging losses during the intake/exhaust stroke. The use of a reformulated gasoline containing 10% ethanol resulted in a 15% decrease in HC and a 29% decrease in CO emissions, on average. Increasing oil content of 2-stroke engine fuels results in a substantial increase of PM2.5 emissions as well as smaller increases in HC and CO emissions. Results from this study enhance existing emission inventories and appear to validate predicted improvements to ambient air quality through implementation of new phase-2 handheld emission standards.  相似文献   

4.
ABSTRACT

The introduction of reformulated gasolines significantly reduced exhaust hydrocarbon (HC) mass emissions, but few data are available concerning how these new fuels affect exhaust reactivity. Similarly, while it is well established that high-emitting vehicles contribute a significant portion of total mobile source HC mass emissions, it is also important to evaluate the exhaust reactivity from these vehicles. The objective of this study was to evaluate the relative influence on in-use vehicle exhaust reactivity of three critical factors: fuel, driving cycle, and vehicle emission status. Nineteen in-use vehicles were tested with seven randomly assigned fuel types and two driving cycles: the Federal Test Procedure (FTP) and the Unified Cycle (UC). Total exhaust reactivity was not statistically different between the FTP and UC cycles but was significantly affected by fuel type. On average, the exhaust reactivity for California Phase 2 fuel was the lowest (16 % below the highest fuel type) among the seven fuels tested for cold start emissions. The average exhaust reactivity for high-emitting vehicles was significantly higher for hot stabilized (11%) and hot start (15%) emissions than for low-emitting vehicles. The exhaust reactivities for the FTP and UC cycles for light-end HCs and carbonyls were significantly different for the hot stabilized mode. There was a significant fuel effect on the mean specific reactivity (SR) for the mid-range HCs, but not for light-end HCs or carbonyls, while vehicle emission status affected the mean SR for all three HC compound classes.  相似文献   

5.
Abstract

In this paper, the deterioration of catalysts in small, four-stroke, spark-ignition engines is described. The laboratory testing performed followed a proven test method that mimics the lifetime of a small air-cooled utility engine operating under normal field conditions. The engines used were single-cylinder, 6.5-hp, side-valve engines. These engines have a nominal 125-hr lifetime. The effectiveness of the catalysts was determined by testing exhaust emissions before and after the catalyst to determine the catalyst’s efficiency. This was done several times during the lifetime of the engines to determine the deterioration in the performance of the catalysts at lowering pollutant emissions. Additional testing was performed on the catalysts to determine wear patterns, contamination, and recoverable activity. The results indicate that considerable catalyst deterioration is occurring over the lifetime of the engine. The results reveal that soot buildup, poisons, and active surface loss appear to be the contributing factors to the deterioration. These results were determined after analyzing the exhaust emissions data, scanning electron microscope results analysis, and the impact of regeneration attempts. An ANOVA statistical analysis was performed, and it was determined that the emissions are also impacted, to some degree, by time and the engine itself.  相似文献   

6.
The formation of chemical oxidants, particularly ozone, in Mexico City were studied using a newly developed regional chemical/dynamical model (WRF-Chem). The magnitude and timing of simulated diurnal cycles of ozone (O3), carbon monoxide (CO) and nitrogen oxides (NOx), and the maximum and minimum O3 concentrations are generally consistent with surface measurements. Our analysis shows that the strong diurnal cycle in O3 is mainly attributable to photochemical variations, while diurnal cycles of CO and NOx mainly result from variations of emissions and boundary layer height. In a sensitivity study, oxidation reactions of aromatic hydrocarbons (HCs) and alkenes yield highest peak O3 production rates (20 and 18 ppbv h−1, respectively). Alkene oxidations, which are generally faster, dominate in early morning. By late morning, alkene concentrations drop, and oxidations of aromatics dominate, with lesser contributions from alkanes and CO. The sensitivity of O3 concentrations to NOx and HC emissions was assessed. Our results show that daytime O3 production is HC-limited in the Mexico City metropolitan area, so that increases in HC emissions increase O3 chemical production, while increases in NOx emissions decrease O3 concentrations. However, increases in both NOx and HC emissions yield even greater O3 increases than increases in HCs alone. Uncertainties in HC emissions estimates give large uncertainties in calculated daytime O3, while NOx emissions uncertainties are less influential. However, NOx emissions are important in controlling O3 at night.  相似文献   

7.
Abstract

In Mexico City, the use and composition of fuels determine that carbon monoxide (CO) comes mostly from mobile sources, and sulfur dioxide (SO2) from fixed and mobile sources. By simultaneously measuring hydrocarbons (HC), CO, and SO2 in the atmosphere of Mexico City, the relative amounts coming from different sources can be estimated. Assuming that some HC are emitted proportionally to CO emissions, we can establish that [HC]1= m1? [CO], where the proportionality constant ml corresponds to the ratio of emissions factor for HC and CO in mobile sources. Similarly for fuels containing sulfur, it can be assumed that [HC]2 = m2 ? [SO2]. In this way, the total HC are [HC]total=[HC]0+ ml ? [CO]+ m2 ? [SO2], where [HC]0 corresponds mainly to other sources like solvent evaporation, gas consumption, and natural emissions. In this way, it can be estimated that in Mexico City 75% of average HC comes from mobile sources, 5% from sulfur-related sources, and 19% from natural sources and solvent evaporation. Compared with the HC/CO ratio measured in the exhaust pipe of vehicles, we estimated that 70% of HC emitted from mobile sources are evaporative losses, and only 30% come through the exhaust system.  相似文献   

8.
Abstract

Refineries are a source of emissions of volatile hydrocarbons that contribute to the formation of smog and ozone. Fugitive emissions of hydrocarbons are difficult to measure and quantify. Currently these emissions are estimated based on standard emission factors for the type and use of equipment installed. Differential absorption light detection and ranging (DIAL) can remotely measure concentration profiles of hydrocarbons in the atmosphere up to several hundred meters from the instrument. When combined with wind speed and direction, downwind vertical DIAL scans can be used to calculate mass fluxes of the measured gas leaving the site. Using a mobile DIAL unit, a survey was completed at a Canadian refinery to quantify fugitive emissions of methane, C2+ hydrocarbons, and benzene and to apportion the hydrocarbon emissions to the various areas of the refinery. Refinery fugitive emissions as measured with DIAL during this demonstration study were 1240 kg/hr of C2+ hydrocarbons, 300 kg/hr of methane, and 5 kg/hr of benzene. Storage tanks accounted for over 50% of the total emissions of C2+ hydrocarbons and benzene. The coker area and cooling towers were also significant sources. The C2+ hydrocarbons emissions measured during the demonstration amounted to 0.17% of the mass of the refinery hydrocarbon throughput for that period. If the same loss were repeated throughout the year, the lost product would represent a value of US$3.1 million/yr (assuming US$40/bbl). The DIAL-measured hourly emissions of C2+ hydrocarbons were 15 times higher than the emission factor estimates and gave a different perspective on which areas of the refinery were the main source of emissions. Methods, such as DIAL, that can directly measure fugitive emissions would improve the effectiveness of efforts to reduce emissions, quantify the reduction in emissions, and improve the accuracy of emissions data that are reported to regulators and the public.  相似文献   

9.
The formation of O3 and other photochemically generated compounds has been modelled for the region downwind of London, during the slow easterly airflow and other conditions associated with a midsummer anticyclone. The model contains a comprehensive chemical mechanism, including the emissions of 37 hydrocarbons (HCs) and treats HC degradation explicitly in over 300 reactions. As a result it has been possible to disaggregate the production of O3 amongst the various HCs present in the model, and the percentage of the O3 production which can be attributed to each HC is therefore known. These results have been used, in conjunction with the emissions inventory, to attribute the O3 production to the various sources of HCs. By further study the number of molecules of O3 which are produced by each HC molecule have also been elucidated. The significance of the results both to control strategies for O3 formation and to the representation of photochemical O3 production in computational models is discussed.  相似文献   

10.
ABSTRACT

We examine the life cycles of gasoline, diesel, compressed natural gas (CNG), and ethanol (C2H5OH)-fueled internal combustion engine (ICE) automobiles. Port and direct injection and spark and compression ignition engines are examined. We investigate diesel fuel from both petroleum and biosources as well as C2H5OH from corn, herbaceous bio-mass, and woody biomass. The baseline vehicle is a gasoline-fueled 1998 Ford Taurus. We optimize the other fuel/powertrain combinations for each specific fuel as a part of making the vehicles comparable to the baseline in terms of range, emissions level, and vehicle lifetime. Life-cycle calculations are done using the economic input-output life-cycle analysis (EIO-LCA) software; fuel cycles and vehicle end-of-life stages are based on published model results.

We find that recent advances in gasoline vehicles, the low petroleum price, and the extensive gasoline infrastructure make it difficult for any alternative fuel to become commercially viable. The most attractive alternative fuel is compressed natural gas because it is less expensive than gasoline, has lower regulated pollutant and toxics emissions, produces less greenhouse gas (GHG) emissions, and is available in North America in large quantities. However, the bulk and weight of gas storage cylinders required for the vehicle to attain a range comparable to that of gasoline vehicles necessitates a redesign of the engine and chassis. Additional natural gas transportation and distribution infrastructure is required for large-scale use of natural gas for transportation. Diesel engines are extremely attractive in terms of energy efficiency, but expert judgment is divided on whether these engines will be able to meet strict emissions standards, even with reformulated fuel. The attractiveness of direct injection engines depends on their being able to meet strict emissions standards without losing their greater efficiency. Biofuels offer lower GHG emissions, are sustainable, and reduce the demand for imported fuels. Fuels from food sources, such as biodiesel from soybeans and C2H5OH from corn, can be attractive only if the co-products are in high demand and if the fuel production does not diminish the food supply. C2H5OH from herbaceous or woody biomass could replace the gasoline burned in the light-duty fleet while supplying electricity as a co-product. While it costs more than gasoline, bioethanol would be attractive if the price of gasoline doubled, if significant reductions in GHG emissions were required, or if fuel economy regulations for gasoline vehicles were tightened.  相似文献   

11.
ABSTRACT

Profiles of the sources of nonmethane organic compounds (NMOCs) were developed for emissions from vehicles, petroleum fuels (gasoline, liquefied petroleum gas [LPG], and natural gas), a petroleum refinery, a smelter, and a cast iron factory in Cairo, Egypt. More than 100 hydrocarbons and oxygenated hydrocarbons were tentatively identified and quantified. Gasoline-vapor and whole-gasoline profiles could be distinguished from the other profiles by high concentrations of the C5 and C6 saturated hydrocarbons. The vehicle emission profile was similar to the whole-gasoline profile, with the exception of the unsaturated and aromatic hydrocarbons, which were present at higher concentrations in the vehicle emission profile. High levels of the C2-C4 saturated hydrocarbons, particularly n-butane, were characteristic features of the petroleum refinery emissions. The smelter and cast iron factory emissions were similar to the refinery emissions; however, the levels of benzene and toluene were greater in the former two sources. The LPG and natural gas emissions contained high concentrations of n-butane and ethane, respectively. The NMOC source profiles for Cairo were distinctly different from profiles for U.S. sources, indicating that NMOC source profiles are sensitive to the particular composition of petroleum fuels that are used in a location.  相似文献   

12.
Experiments were conducted on a 4-cylinder direct-injection diesel engine using ultralow sulfur diesel blended with biodiesel and ethanol to investigate the gaseous emissions of the engine under five engine loads at the maximum torque engine speed of 1800 rev min?1. Four biodiesel blended fuels and four ethanol blended fuels with oxygen concentrations of 2%, 4%, 6% and 8% were used. With the increase of oxygen content in the blended fuels, the brake thermal efficiency improves slightly.For the diesel-biodiesel fuels, the brake specific HC and CO emissions decrease while the brake specific NOx and NO2 emissions increase. The emissions of formaldehyde, 1,3-butadiene, toluene, xylene and overall BTX (benzene, toluene, xylene) in general decrease, however, acetaldehyde and benzene emissions increase. For the diesel-ethanol fuels, the brake specific HC and CO emissions increase significantly at low engine load, NOx emission decreases at low engine load but increases at high engine load. The emissions of benzene and BTX vary with engine load and ethanol content. Similar to the biodiesel-diesel fuels, the formaldehyde, 1,3-butadiene, toluene and xylene emissions decrease while the acetaldehyde and NO2 emissions increase. Despite having the same oxygen contents in the blended fuels, there are significant differences in the gaseous emissions between the biodiesel-diesel blends and the ethanol-diesel blends.  相似文献   

13.
14.
Experiments were carried out on a diesel engine operating on Euro V diesel fuel, pure biodiesel and biodiesel blended with methanol. The blended fuels contain 5%, 10% and 15% by volume of methanol. Experiments were conducted under five engine loads at a steady speed of 1800 rev min−1 to assess the performance and the emissions of the engine associated with the application of the different fuels. The results indicate an increase of brake specific fuel consumption and brake thermal efficiency when the diesel engine was operated with biodiesel and the blended fuels, compared with the diesel fuel. The blended fuels could lead to higher CO and HC emissions than biodiesel, higher CO emission but lower HC emission than the diesel fuel. There are simultaneous reductions of NOx and PM to a level below those of the diesel fuel. Regarding the unregulated emissions, compared with the diesel fuel, the blended fuels generate higher formaldehyde, acetaldehyde and unburned methanol emissions, lower 1,3-butadiene and benzene emissions, while the toluene and xylene emissions not significantly different.  相似文献   

15.
Abstract

Understanding ozone response to its precursor emissions is crucial for effective air quality management practices. This nonlinear response is usually simulated using chemical transport models, and the modeling results are affected by uncertainties in emissions inputs. In this study, a high ozone episode in the southeastern United States is simulated using the Community Multiscale Air Quality (CMAQ) model. Uncertainties in ozone formation and response to emissions controls due to uncertainties in emission rates are quantified using the Monte Carlo method. Instead of propagating emissions uncertainties through the original CMAQ, a reduced form of CMAQ is formulated using directly calculated first- and second-order sensitivities that capture the nonlinear ozone concentration-emission responses. This modification greatly reduces the associated computational cost. Quantified uncertainties in modeled ozone concentrations and responses to various emissions controls are much less than the uncertainties in emissions inputs. Average uncertainties in modeled ozone concentrations for the Atlanta area are less than 10% (as measured by the inferred coefficient of variance [ICOV]) even when emissions uncertainties are assumed to vary between a factor of 1.5 and 2. Uncertainties in the ozone responses generally decrease with increased emission controls. Average uncertainties (ICOV) in emission-normalized ozone responses range from 4 to 22%, with the smaller being associated with controlling of the relatively certain point nitrogen oxide (NOx) emissions and the larger resulting from controlling of the less certain mobile NOx emissions. These small uncertainties provide confidence in the model applications, such as in performance evaluation, attainment demonstration, and control strategy development.  相似文献   

16.
An ambient air monitoring program to characterize airborne emissions from the Exxon petroleum refinery at Benicia, California was conducted during September 8–22, 1975. Ground level sampling facilities and an instrumented aircraft provided an integrated, three-dimensional monitoring network. Measurements made during the study included ozone, oxides of nitrogen, methane, carbon monoxide, individual C2-C6 hydrocarbons, halocarbons, condensation nuclei, visual distance and various meteorological parameters. The study focused on three major areas: (1) the characterization of gaseous components within the refinery effluent, especially non-methane hydrocarbons and ozone, (2) natural sunlight bag irradiation experiments to determine the ozone forming potential of refinery emissions, and (3) an investigation of changes in plume chemistry as refinery emissions were transported downwind.  相似文献   

17.
Germany     
ABSTRACT

The 1988 Alternative Motor Fuels Act and the 1990 Clean Air Act Amendments require examination of the potential to favorably influence air quality by changing the composition of motor vehicle fuels. Motor vehicle tailpipe and evaporative emissions were characterized using laboratory simulations of roadway driving conditions and a variety of vehicle-fuel technologies (reformulated gasoline (RFG), methanol (M85), ethanol (E85), and natural gas (CNG)). Speciated organic compound (with Carter MIR ozone potential), CO, and NOx emission rates and fuel economy were characterized. The Carter MIR ozone potential of combined Federal Test Procedure (FTP) tailpipe and evaporative emissions was reduced more than 90% with CNG relative to RFG, M85, and E85 fuels. FTP toxic compound emissions (benzene, formaldehyde, acetalde-hyde, and 1,3-butadiene) were greater with M85 and E85 fuels than with RFG fuel, and less with CNG fuel than RFG fuel. The most abundant toxic compound was benzene with RFG fuel, formaldehyde with M85 fuel, and acetaldehyde with E85 fuel. FTP MPG fuel economies were reduced with M85 and E85 fuels relative to RFG fuel, consistent with their lower BTU/gal. Energy efficiencies (BTU/mi) were improved with all the alternative fuels relative to RFG. Carter MIR ozone potential was generally reduced with the alternative fuels relative to RFG fuel under REP05 (high speeds and acceleration rates) driving conditions (most significantly with CNG). Toxic aldehyde emissions were reduced under REP05 conditions relative to FTP conditions with all the tested fuels, and toxic benzene emissions were elevated under high acceleration conditions.  相似文献   

18.
The body of information presented in this paper is directed towards engineers in the field of environmental sciences involved in measuring and/or evaluating the emissions from a variety of diesel engines or vehicles. This paper summarizes recent data obtained by EPA on identification and quantification of different emissions (i.e. characterization) from a variety of diesel engines.

Extensive work has been done comparing emissions from some light duty diesel and gasoline passenger cars. The work on the diesel vehicles was expanded to include tests with five different diesel fuels to determine how fuel composition affects emissions. This work showed that use of a poorer quality fuel frequently made emissions worse. The investigation of fuel composition continued with a project in which specific fuel parameters were systematically varied to determine their effect on emissions. EPA is presently testing a variety of fuels derived from coal and oil shale to determine their effects on emissions.

EPA has also tested a heavy duty Volvo diesel bus engine designed to run on methanol and diesel fuel, each injected through its own injection system. The use of the dual fuel resulted in a reduction in particulates and NO x but an increase in HC and CO compared to a baseline Volvo diesel engine running on pure diesel fuel.

Finally, some Ames bioassay tests have been performed on samples from the diesel passenger cars operated on various fuels and blends. An increase in Ames test response (mutagenicity) was seen when the higher aromatic blend was used and also when a commercial cetane improver was used. Samples from the Volvo diesel bus engine fueled with methanol and diesel fuel showed that use of a catalyst increased the Ames response.  相似文献   

19.
Diesel engine emissions are composed of a long list of organic compounds, ranging from C2 to C12+, and coming from the hydrocarbons partially oxidized in combustion or produced by pyrolisis. Many of these are considered as ozone precursors in the atmosphere, since they can interact with nitrogen oxides to produce ozone under atmospheric conditions in the presence of sunlight. In addition to problematic ozone production, Brookes, P., and Duncan, M. [1971. Carcinogenic hydrocarbons and human cells in culture. Nature.] and Heywood, J. [1988. Internal Combustion Engine Fundamentals.Mc Graw-Hill, ISBN 0-07-1000499-8.] determined that the polycyclic aromatic hydrocarbons present in exhaust gases are dangerous to human health, being highly carcinogenic.The aim of this study was to identify by means of gas chromatography the amount of each hydrocarbon species present in the exhaust gases of diesel engines operating with different biodiesel blends. The levels of reactive and non-reactive hydrocarbons present in diesel engine exhaust gases powered by different biodiesel fuel blends were also analyzed.Detailed speciation revealed a drastic change in the nature and quantity of semi-volatile compounds when biodiesel fuels are employed, the most affected being the aromatic compounds. Both aromatic and oxygenated aromatic compounds were found in biodiesel exhaust. Finally, the conservation of species for off-side analysis and the possible influence of engine operating conditions on the chemical characterization of the semi-volatile compound phase are discussed.The use of oxygenated fuel blends shows a reduction in the Engine-Out emissions of total hydrocarbons. But the potential of the hydrocarbon emissions is more dependent on the compositions of these hydrocarbons in the Engine-Out, to the quantity; a large percent of hydrocarbons existing in the exhaust, when biodiesel blends are used, are partially burned hydrocarbons, and are interesting as they have the maximum reactivity, but with the use of pure biodiesel and diesel, the most hydrocarbons are from unburned fuel and they have a less reactivity. The best composition in the fuel, for the control of the hydrocarbon emissions reactivity, needs to be a fuel with high-saturated fatty acid content.  相似文献   

20.
A three-dimensional global chemical tracer model and a radiation transfer model have been used to study the role of NOx emissions for radiative forcing of climate. Through production of tropospheric O3, NOx emissions lead to positive radiative forcing and warming. But by affecting the concentration of OH radicals, NOx also reduces the levels of CH4, thereby giving negative forcing and cooling. The lifetime of NOx varies from hours to days, giving large spatial variations in the levels of NOx. We have selected geographical regions representing different chemical and physical conditions, and chemical and radiative effects of reducing NOx emissions by 20% in each region are studied. Due to nonlinearities in the O3 chemistry as well as differences in convective activity, there are large geographical differences in the effect of NOx on O3 as well as variations in the annual profile of the changes. The effect of NOx emissions on methane is also found to depend on the localisation of the emissions. The calculated ozone and methane forcing are of similar magnitude but of opposite sign. The methane effect acts on a global scale with a delay of approximately a decade, while the ozone effect is of regional character and occurs during weeks.  相似文献   

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