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1.
Because of the considerable uncertainties associated with modeling complex ecosystem processes, it is essential that every effort be made to test model performance prior to relying on model projections for assessment of future surface water chemical response to environmental perturbation. Unfortunately, long-term chemical data with which to validate model performance are seldom available. The authors present here an evaluation of historical acidification of lake waters in the northeastern United States, and compare historical changes in a set of lakes to hindcasts from the same watershed model (MAGIC) used to estimate future changes in response to acidic deposition. The historical analyses and comparisons with MAGIC model hindcasts and forecasts of acid-base response demonstrate that the acidic and low-ANC lakes in this region are responsive to strong acid inputs. However, the model estimates suggest lakewater chemistry is more responsive to atmospheric inputs of sulfur than do the estimates based on paleolimnological historical analyses. A 'weight-of-evidence approach' that incorporates all available sources of information regarding acid-base response provides a more reasonable estimate of future change than an approach based on model projections alone. The results of these analyses have important implications for predicting future surface water chemical change in response to acidic deposition, establishing critical loads of atmospheric pollutants, and other environmental assessment activities where natural variation often exceeds the trends under investigation (high noise-to-signal ratio). Under these conditions, it is particularly important to evaluate future model projections in light of historical trends data.  相似文献   

2.
This work examines the performance of the CHIMERE photochemical model in simulating ozone and nitrogen dioxide in Portugal over a long-term summer period. The analysis focuses on comparisons against the available measurements during the 2001 summer season. The meteorological forcing of the model is given by the European Centre for Medium-Range Weather Forecasts (ECMWF), and the emission inventory used was obtained with a top-down methodology updated for the simulation year.Despite the coarse resolution of the meteorological data, the complex topography and coastal location of Portugal, the results obtained show that the modelling system is able to reproduce the nitrogen dioxide and ozone episodes that occurred during the simulated summer period. Mean error and correlation improve when considering the sum of photo oxidant instead of individual pollutants, indicating that a significant part of the model error is due to either the lack of representativeness of monitoring stations or to inaccuracies in the emission inventory.  相似文献   

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Nitrogen dioxide (NO2) plays a key role in the chemistry of the atmosphere and is emitted mainly by combustion processes. These emissions have been increasing over India over the past few years due to rapid economic growth and yet there are very few systematic ground based observations of NO2 over this region. We thus take recourse to satellite data and compare tropospheric NO2 column abundances simulated by a chemical transport model, MOZART, with data from the Global Ozone Monitoring Experiment (GOME) for a few locations in India that have seen a rapid economic growth in the last decade. The model generally simulates higher columnar abundances of NO2 compared to GOME observations and does not reproduce the features of the observed seasonal behaviour. The combined uncertainties of the emission inventory and retrieval of the satellite data could be contributing factors to the discrepancies. It may be thus worthwhile to develop emission inventories for India at a higher resolution to include local level activity data. The ten year data (1996–2006) from GOME and SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) show increasing trends for Indian cities where rapid industrial and vehicular traffic growth has been observed during this period.  相似文献   

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This study aims to evaluate near surface ozone simulated with the modelling system RegCM3/CAMx against ozone measurements from the EMEP database for the recent decade 1991–2000. The RegCM3/CAMx simulations were performed on a 50 km × 50 km grid over Europe driven either by ERA-40 reanalysis (hereafter referred as ERA simulation) or the global circulation model (GCM) ECHAM5 (hereafter referred as ECHAM simulation). A set of statistical metrics is used for the model evaluation, including temporal correlation coefficient, the ratio of the standard deviations and the bias of simulated versus observed values. Overall, a good agreement is found for both ERA and ECHAM simulations at the majority of the selected EMEP stations in all metrics throughout the year based either on monthly or daily ozone values. Based on these results, it is assessed that the modelling system RegCM3/CAMx is suitable to be used for present and future regional climate-air quality simulations with emphasis on near surface ozone. The ERA simulations reproduce more accurately the observed ozone values in comparison to ECHAM simulations because the meteorology of the ERA experiment is closer to real atmospheric conditions than the GCM based experiment. On a seasonal basis, both ERA and ECHAM simulations exhibit a seasonally dependent bias, with winter and spring ozone values being generally under-estimated by the model and summer and autumn values being slightly overestimated. This seasonally dependent bias is also evident from median and peak midday ozone values. However, the highest observed midday ozone peaks in summer, with values higher than 80 ppbv, could not be captured either by ERA or ECHAM simulations. An analysis of day-time and night-time ERA and ECHAM modelled ozone values shows that CAMx performs better during the day-time.  相似文献   

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The prediction of future air quality and its responses to emission control strategies at national and state levels requires a reliable model that can replicate atmospheric observations. In this work, the Mesoscale Model (MM5) and the Community Multiscale Air Quality Modeling (CMAQ) system are applied at a 4-km horizontal grid resolution for four one-month periods, i.e., January, June, July, and August in 2002 to evaluate model performance and compare with that at 12-km. The evaluation shows skills of MM5/CMAQ that are overall consistent with current model performance. The large cold bias in temperature at 1.5 m is likely due to too cold soil initial temperatures and inappropriate snow treatments. The large overprediction in precipitation in July is due likely to too frequent afternoon convective rainfall and/or an overestimation in the rainfall intensity. The normalized mean biases and errors are ?1.6% to 9.1% and 15.3–18.5% in January and ?18.7% to ?5.7% and 13.9–20.6% in July for max 1-h and 8-h O3 mixing ratios, respectively, and those for 24-h average PM2.5 concentrations are 8.3–25.9% and 27.6–38.5% in January and ?57.8% to ?45.4% and 46.1–59.3% in July. The large underprediction in PM2.5 in summer is attributed mainly to overpredicted precipitation, inaccurate emissions, incomplete treatments for secondary organic aerosols, and model difficulties in resolving complex meteorology and geography. While O3 prediction shows relatively less sensitivity to horizontal grid resolutions, PM2.5 and its secondary components, visibility indices, and dry and wet deposition show a moderate to high sensitivity. These results have important implications for the regulatory applications of MM5/CMAQ for future air quality attainment.  相似文献   

9.
Large-eddy simulation (LES) is used to simulate neutral turbulent boundary-layer flow over a rough two-dimensional sinusoidal hill. Three different subgrid-scale (SGS) models are tested: (a) the standard Smagorinsky model with a wall-matching function, (b) the Lagrangian dynamic model, and (c) the recently developed scale-dependent Lagrangian dynamic model [Stoll, R., Porté-Agel, F., 2006. Dynamic subgrid-scale models for momentum and scalar fluxes in large-eddy simulation of neutrally stratified atmospheric boundary layers over heterogeneous terrain. Water Resources Research 42, W01409. doi:10.1029/2005WR003989]. The simulation results obtained with the different models are compared with turbulence statistics obtained from experiments conducted in the meteorological wind tunnel of the AES (Atmospheric Environment Service, Canada) [Gong, W., Taylor, P.A., Dörnbrack, A., 1996. Turbulent boundary-layer flow over fixed aerodynamically rough two-dimensional sinusoidal waves. Journal of Fluid Mechanics 312, 1–37]. We find that the scale-dependent dynamic model is able to account, without any tuning, for the local changes in the eddy-viscosity model coefficient. It can also capture the scale dependence of the coefficient associated with regions of the flow with strong mean shear and flow anisotropy. As a result, the scale-dependent dynamic model yields results that are more realistic than the ones obtained with the scale-invariant Lagrangian dynamic model.  相似文献   

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The influence of chemical boundary conditions (BC) on the response of the Community Multiscale Air Quality (CMAQ) model over the Iberian Peninsula was investigated in this study. Three strategies to supply boundary conditions in the context of the Integrated Assessment Modelling System for the Iberian Peninsula (SIMCA) were tested. Alternative methods consist in providing BC from (1) fixed, time-independent, concentration profiles, (2) concentrations predicted in a CMAQ mother domain (48 km, 1 h resolution) and (3) concentration values from the GEOS-Chem chemical-transport global model (2 × 2.5°, 3 h resolution). High resolution (3 km) simulated concentrations of the main pollutants (NO2, NO, SO2, O3, PM10 and PM2.5) were compared through a comprehensive statistical analysis including observational data from 165 monitoring stations all over the Iberian Peninsula. It was found that model sensitivity to BC for nitrogen and sulphur oxides was limited, being restricted to the vicinity of model boundaries. However, significant domain-wide differences were found when modelling ozone and PM depending on the BC provided to run the tests. Although model performance was affected by spatial and seasonal factors, the results indicate that model-derived, dynamic BC improved CMAQ predictions when compared to those based on static concentrations prescribed in the boundaries. Aggregated statistics suggest that the GEOS-Chem produced the best results for O3 and PM2.5 while NO2 and PM10 were slightly better predicted under the CMAQ nesting approach. Besides the statistical evaluation some other relevant issues in the context of Integrated Assessment Modelling (IAM) are discussed to gain a better insight into the suitability of the methods analyzed and limitations of downscaling methods. Despite being useful to get a better understanding of the role of BC in SIMCA, this study contributed to highlight model deficiencies and therefore to point out future research needs to improve IAM activities in the Iberian Peninsula.  相似文献   

12.
The results of application of two nested Eulerian atmospheric transport models for investigation of airborne heavy metal pollution are presented. The distribution and deposition over Europe and Baltic Sea region were simulated for Pb, Cd and Zn for 2 two-months periods: June–July 1997 and February–March 1998. The European-wide calculations were made with the ADOM model from the GKSS Research Centre, and the Baltic regional calculations were made with the HILATAR model from the Finnish Meteorological Institute. The one-way 3-D nesting was used: hourly concentrations from the ADOM model were used by the HILATAR as vertically resolved boundary conditions. Input data for both models were taken from the weather forecast model HIRLAM and UBA/TNO emission inventory. This allows interpreting of some diversity in the calculation results in terms of different internal parameterization and spatial resolution of the models. Simulation results were compared with high-resolution atmospheric measurements carried out at four stations in the southern part of the Baltic Sea for the same period. Manifesting quite good agreement with observations, the models missed several high deposition events of Cd observed at coastal station Hel. Study of this phenomenon enabled to build a 2-D probability function for potential location of the unknown Cd source.  相似文献   

13.
Environmental Science and Pollution Research - Climate change affects air quality and people’s health. Therefore, accurate prediction of future climate change is of great significance for...  相似文献   

14.
In response to increasing trends in sulfur deposition in Northeast Asia, three countries in the region (China, Japan, and Korea) agreed to devise abatement strategies. The concepts of critical loads and source?Creceptor (S?CR) relationships provide guidance for formulating such strategies. Based on the Long-range Transboundary Air Pollutants in Northeast Asia (LTP) project, this study analyzes sulfur deposition data in order to optimize acidic loads over the three countries. The three groups involved in this study carried out a full year (2002) of sulfur deposition modeling over the geographic region spanning the three countries, using three air quality models: MM5-CMAQ, MM5-RAQM, and RAMS-CADM, employed by Chinese, Japanese, and Korean modeling groups, respectively. Each model employed its own meteorological numerical model and model parameters. Only the emission rates for SO2 and NOx obtained from the LTP project were the common parameter used in the three models. Three models revealed some bias from dry to wet deposition, particularly the latter because of the bias in annual precipitation. This finding points to the need for further sensitivity tests of the wet removal rates in association with underlying cloud?Cprecipitation physics and parameterizations. Despite this bias, the annual total (dry plus wet) sulfur deposition predicted by the models were surprisingly very similar. The ensemble average annual total deposition was 7,203.6?±?370 kt S with a minimal mean fractional error (MFE) of 8.95?±?5.24?% and a pattern correlation (PC) of 0.89?C0.93 between the models. This exercise revealed that despite rather poor error scores in comparison with observations, these consistent total deposition values across the three models, based on LTP group's input data assumptions, suggest a plausible S?CR relationship that can be applied to the next task of designing cost-effective emission abatement strategies.  相似文献   

15.
Two-year CMAQ simulations of gases and aerosols over the southeast are evaluated using SEARCH observations for 2000 and 2001, both by direct comparison to observations and by projecting both datasets to the factor space using the Positive Matrix Factorization (PMF) model. Model performance for secondary species (sulfate, ozone) is generally better than for primary species (EC, CO). Nitrate concentrations are overestimated, mainly due to wintertime over-partitioning to the particulate phase. Projecting both observed and simulated constituents to the factor space using PMF, four common factors are resolved for each surface site (two urban sites and two rural sites). The resolved factors include (1) secondary sulfate, (2) secondary nitrate, (3) a fresh motor vehicle factor characterized by EC, OC, CO, NO and NOy, and (4) a mixed factor characterized by EC, OC, and CO. Performance for the sulfate and nitrate factors follow that of the corresponding driving species, while the motor vehicle and “mixed” factors exhibit performance corresponding to that of primary species. Comparing observations and CMAQ simulations in the projected space allow for an evaluation of the co-variability between species, an indicator of source impacts. The fact that similar factors were resolved by PMF from both the observations and the CMAQ simulations suggests that temporal processes related to emissions from specific source categories, as well as the subsequent dispersion and reactivity, are well captured by the CMAQ model. The ability to identify additional factors can be enhanced by adding tracer species in CMAQ simulations.  相似文献   

16.
An ozone pollution episode typically at the mesoscale is studied for the period 17–20 July 1996 in the northern half of France. This episode has been documented through extra stations supplementing the regular French network in the southwest of the Paris region at large: the ozone threshold value of 90 ppb has been observed to be exceeded only at downwind rural stations at distances ranging between 25 and 110 km from downtown Paris. This episode has been simulated with the mesoscale model Meso-NH-C in which the meteorological model Meso-NH is coupled on-line with a chemistry module. Various assumptions are presented which must be made in order to run Meso-NH-C:  e.g. reduction of the chemical scheme to reduce the computational costs or definition of procedures to fill in the lack of emission inventory data. Meso-NH appears to realistically simulate the position, extent, average and peak ozone values within the pollution plume. Sensitivity analyses emphasize, in particular, the need for accurate simulation of the wind field to capture correct characteristics of this plume.  相似文献   

17.
In order to investigate benzo(a)pyrene (B(a)P) concentrations in ambient air in Europe and the respective deposition fields an expanded version of the Community Multiscale Air Quality (CMAQ) Modelling system has been used to simulate these fields for the years 2000 and 2001. Significant differences exist between different regions in Europe and between winter and summer concentrations. Modelled B(a)P concentrations are highest in Central Europe, South Ukraine and around Moscow. Wet deposition shows mainly the same regional distribution as the concentrations. Simulated concentrations and depositions are compared to measurements at selected sites of the EMEP network and of the German Federal Environmental Agencies. The measurements are on average underestimated by 50%. The temporal evolution and the regional distribution of B(a)P are captured by the model. In the approach presented here, particle bound B(a)P undergoes degradation by reactions with ozone. In order to assess the importance of the degradation process the results are compared to a model run where no degradation of particle bound B(a)P is considered. It was found that the inclusion of heterogeneous reactions of B(a)P with ozone results in a reduction of the modelled air concentration by approx. a factor of 5.  相似文献   

18.
Transport affects climate directly and indirectly through mechanisms that operate on very different timescales and cause both warming and cooling. We calculate contributions to the historical development in global mean temperature for the main transport sectors (road transport, aviation, shipping and rail) based on estimates of historical emissions and by applying knowledge about the various forcing mechanisms from detailed studies. We also calculate the development in future global mean temperature for four transport scenarios consistent with the IPCC SRES scenarios, one mitigation scenario and one sensitivity test scenario. There are large differences between the transport sectors in terms of sign and magnitude of temperature effects and with respect to the contributions from the long- and short-lived components. Since pre-industrial times, we calculate that transport in total has contributed 9% of total net man-made warming in the year 2000. The dominating contributor to warming is CO2, followed by tropospheric O3. By sector, road transport is the largest contributor; 11% of the warming in 2000 is due to this sector. Likewise, aviation has contributed 4% and rail ~1%. Shipping, on the other hand, has caused a net cooling up to year 2000, with a contribution of ?7%, due to the effects of SO2 and NOx emissions. The total net contribution from the transport sectors to total man-made warming is ~15% in 2050, and reaches 20% in 2100 in the A1 and B1 scenarios. For all scenarios and throughout the century, road transport is the dominating contributor to warming. Due to the anticipated reduction in sulphur content of fuels, the net effect of shipping changes from cooling to warming by the end of the century. Significant uncertainties are related to the estimates of historical and future net warming mainly due to cirrus, contrails and aerosol effects, as well as uncertainty in climate sensitivity.  相似文献   

19.
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   

20.
Environmental Science and Pollution Research - Anthropogenic activities have increased atmospheric concentrations of greenhouse gas emissions, which have observably increased global temperature....  相似文献   

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