Estimation of mercury emissions from forest fires, lakes, regional and local sources using measurements in Milwaukee and an inverse method

Gaseous elemental mercury is a global pollutant that can lead to serious health concerns via deposition to the biosphere and bio-accumulation in the food chain. Hourly measurements between June 2004 and May 2005 in an urban site (Milwaukee, WI) show elevated levels of mercury in the atmosphere with numerous short-lived peaks as well as longer-lived episodes. The measurements are analyzed with an inverse model to obtain information about mercury emissions. The model is based on high resolution meteorological simulations (WRF), hourly back-trajectories (WRF-FLEXPART) and a chemical transport model (CAMx). The hybrid formulation combining back-trajectories and Eulerian simulations is used to identify potential source regions as well as the impacts of forest fires and lake surface emissions. Uncertainty bounds are estimated using a bootstrap method on the inversions. Comparison with the US Environmental Protection Agency's National Emission Inventory (NEI) and Toxic Release Inventory (TRI) shows that emissions from coal-fired power plants are properly characterized, but emissions from local urban sources, waste incineration and metal processing could be significantly under-estimated. Emissions from the lake surface and from forest fires were found to have significant impacts on mercury levels in Milwaukee, and to be underestimated by a factor of two or more

Satellite-derived land surface parameters for mesoscale modelling of the Mexico City basin

International audienceMesoscale meteorological modelling is an important tool to help understand air pollution and heat island effects in urban areas. Accurate wind simulations are difficult to obtain in areas of weak synoptic forcing. Local factors have a dominant role in the circulation and include land surface parameters and their interaction with the atmosphere. This paper examines an episode during the MCMA-2003 field campaign held in the Mexico City Metropolitan Area (MCMA) in April of 2003. High resolution satellite observations are used to specify the land use, vegetation fraction, albedo and surface temperature in the MM5 model. Making use of these readily available data leads to improved meteorological simulations in the MCMA, both for the wind circulation patterns and the urban heat island. Replacing values previously obtained from land-use tables with actual measurements removes the number of unknowns in the model and increases the accuracy of the energy budget. In addition to improving the understanding of local meteorology, this sets the stage for the use of advanced urban modules

Distinct wind convergence patterns in the Mexico City basin due to the interaction of the gap winds with the synoptic flow

International audienceMexico City lies in a high altitude basin where air quality and pollutant fate is strongly influenced by local winds. The combination of high terrain with weak synoptic forcing leads to weak and variable winds with complex circulation patterns. A gap wind entering the basin in the afternoon leads to very different wind convergence lines over the city depending on the meteorological conditions. Surface and upper-air meteorological observations are analysed during the MCMA-2003 field campaign to establish the meteorological conditions and obtain an index of the strength and timing of the gap wind. A mesoscale meteorological model (MM5) is used in combination with high-resolution satellite data for the land surface parameters and soil moisture maps derived from diurnal ground temperature range. A simple method to map the lines of wind convergence both in the basin and on the regional scale is used to show the different convergence patterns according to episode types. The gap wind is found to occur on most days of the campaign and is the result of a temperature gradient across the southern basin rim which is very similar from day to day. Momentum mixing from winds aloft into the surface layer is much more variable and can determine both the strength of the flow and the pattern of the convergence zones. Northerly flows aloft lead to a weak jet with an east-west convergence line that progresses northwards in the late afternoon and early evening. Westerlies aloft lead to both stronger gap flows due to channelling and winds over the southern and western basin rim. This results in a north-south convergence line through the middle of the basin starting in the early afternoon. Improved understanding of basin meteorology will lead to better air quality forecasts for the city and better understanding of the chemical regimes in the urban atmosphere

Distinct wind convergence patterns due to thermal and momentum forcing of the low level jet into the Mexico City basin

International audienceMexico City lies in a high altitude basin where air quality and pollutant fate is strongly influenced by local winds. The combination of high terrain with weak synoptic forcing leads to weak and variable winds with complex circulation patterns. A low level jet entering the basin in the afternoon leads to very different wind convergence lines over the city depending on the meteorological conditions. Surface and upper-air meteorological observations are analysed during the MCMA-2003 field campaign to establish the meteorological conditions and obtain an index of the strength and timing of the jet. A mesoscale meteorological model (MM5) is used in combination with high-resolution satellite data for the land surface parameters and soil moisture maps derived from diurnal ground temperature range. A simple method to map the lines of wind convergence both in the basin and on the regional scale is used to show the different convergence patterns according to episode types. The low level jet is found to occur on most days of the campaign and is primarily due to thermal forcing which is very similar from day to day. Momentum mixing from winds aloft into the surface layer is much more variable and can determine both the strength of the jet and the pattern of the convergence zones. Northerly flows aloft lead to a weak jet with an east-west convergence line that progresses northwards in the late afternoon and early evening. Westerlies aloft lead to stronger jets and a north-south convergence line through the middle of the basin starting in the early afternoon. Improved understanding of basin meteorology will lead to better air quality forecasts for the city and better understanding of the chemical regimes in the urban atmosphere

Characterizing ozone production and response under different meteorological conditions in Mexico City

International audienceTropospheric photochemistry, particularly the formation of ozone (O3), depends not only on pollutant emissions, but also on meteorological conditions. In this study a 3-D chemical transport model CAMx was employed to investigate the O3 formation and its response to emission reductions under three distinctively different meteorological conditions ("Cold Surge", "O3-North" and "O3-South") in the Mexico City Metropolitan Area during the MCMA-2003 field measurement campaign. The O3 formation characteristics and sensitivity to emissions changes were found to be weakly dependent on the meteorological conditions. The evolution of O3 formation and sensitivity were also examined along the photochemical plume transport pathway. The midday O3 production was found to undergo a rapid increase in a narrow range of chemical aging, while plumes in the downwind were characterized with low and constant O3 production, and plumes along their transport pathway were featured by a combination of the two. The O3 formation was more VOC sensitive near the source area, but as the plume became chemically aged, O3 formation became progressively VOC insensitive and more NOx sensitive

Characterizing ozone production in the Mexico City Metropolitan Area: a case study using a chemical transport model

International audienceAn episodic simulation is conducted to characterize ozone (O3) photochemical production and investigate its sensitivity to emission changes of ozone precursors in the Mexico City Metropolitan Area (MCMA) using the Comprehensive Air Quality Model with extensions (CAMx). High Ox (O3+NO2) photochemical production rates of 10?80 ppb/h are predicted due to the high reactivity of volatile organic compounds (VOCs) in which alkanes, alkenes, and aromatics exert comparable contributions. The predicted ozone production efficiency is between 4?10 O3 molecules per NOx molecule oxidized, and increases with VOC-to-NO2 reactivity ratio. Process apportionment analyses indicate significant outflow of pollutants such as O3 and peroxyacetyl nitrate (PAN) from the urban area to the surrounding regional environment. PAN is not in chemical-thermal equilibrium during the photochemically active periods. Sensitivity studies of O3 production suggest that O3 formation in the MCMA urban region with less chemical aging (NOz/NOy3 production and its sensitivities to precursors suggest that midday O3 formation during this episode is VOC sensitive in the urban region on the basis of the current emissions inventory. More episodic studies are needed to construct a comprehensive and representative picture of the O3 production characteristics and its response to emission controls

Evaluation of WRF mesoscale simulations and particle trajectory analysis for the MILAGRO field campaign

Accurate numerical simulations of the complex wind flows in the Mexico City Metropolitan Area (MCMA) can be an invaluable tool for interpreting the MILAGRO field campaign results. This paper uses three methods to evaluate numerical simulations of basin meteorology using the MM5 and WRF models: statistical comparisons with observations, "Concentration Field Analysis" (CFA) using measured air pollutant concentrations, and comparison of flow features using cluster analysis. CFA is shown to be a better indication of simulation quality than statistical metrics, and WRF simulations are shown to be an improvement on the MM5 ones. Comparisons with clusters identifies an under-representation of the drainage flows into the basin and an over-representation of wind shear in the boundary layer. Particle trajectories simulated with WRF-FLEXPART are then used to analyse the transport of the urban plume and show rapid venting and limited recirculation during MILAGRO. Lagrangian impacts were identified at the campaign supersites, and age spectra of the pollutants evaluated at those same sites. The evaluation presented in the paper show that mesoscale meteorological simulations are of sufficient accuracy to be useful for MILAGRO data analysis.National Science Foundation (U.S.) (Award ATM-0511803)National Science Foundation (U.S.) (Award ATM-0810950)National Science Foundation (U.S.) (Award ATM-0810931)Molina Center for Energy and the Environmen

Satellite-derived land surface parameters for mesoscale modelling of the Mexico City basin

Mesoscale meteorological modelling is an important tool to help understand air pollution and heat island effects in urban areas. Accurate wind simulations are difficult to obtain in areas of weak synoptic forcing. Local factors have a dominant role in the circulation and include land surface parameters and their interaction with the atmosphere. This paper examines an episode during the MCMA-2003 field campaign held in the Mexico City Metropolitan Area (MCMA) in April of 2003. Because the episode has weak synoptic forcing, there is the potential for the surface heat budget to influence the local meteorology. High resolution satellite observations are used to specify the land use, vegetation fraction, albedo and surface temperature in the MM5 model. Making use of these readily available data leads to improved meteorological simulations in the MCMA, both for the wind circulation patterns and the urban heat island. Replacing values previously obtained from land-use tables with actual measurements removes the number of unknowns in the model and increases the accuracy of the energy budget. In addition to improving the understanding of local meteorology, this sets the stage for the use of advanced urban modules

Rapid ventilation of the Mexico City basin and regional fate of the urban plume

International audienceUrban areas can be large emitters of air pollutants leading to negative health effects and environmental degradation. The rate of venting of these airsheds determines the pollutant loading for given emission levels, and also determines the regional impacts of the urban plume. Mexico City has approximately 20 million people living in a high altitude basin with air pollutant concentrations above the health limits most days of the year. A mesoscale meteorological model (MM5) and a particle trajectory model (FLEXPART) are used to simulate air flow within the Mexico City basin and the fate of the urban plume during the MCMA-2003 field campaign. The simulated trajectories are validated against pilot balloon and radiosonde trajectories. The residence time of air within the basin and the impacted areas are identified by episode type. Three specific cases are analysed to identify the meteorological processes involved. For most days, residence times in the basin are less than 12 h with little carry-over from day to day and little recirculation of air back into the basin. Very efficient vertical mixing leads to a vertically diluted plume which, in April, is transported predominantly towards the Gulf of Mexico. Regional accumulation was found to take place for some days however, with urban emissions sometimes staying over Mexico for more than 6 days. Knowledge of the residence times, recirculation patterns and venting mechanisms will be useful in guiding policies for improving the air quality of the MCMA

Modelling constraints on the emission inventory and on vertical dispersion for CO and SO₂ in the Mexico City Metropolitan Area using Solar FTIR and zenith sky UV spectroscopy

International audienceEmissions of air pollutants in and around urban areas lead to negative health impacts on the population. To estimate these impacts, it is important to know the sources and transport mechanisms of the pollutants accurately. Mexico City has a large urban fleet in a topographically constrained basin leading to high levels of carbon monoxide (CO). Large point sources of sulfur dioxide (SO2) surrounding the basin lead to episodes with high concentrations. An Eulerian grid model (CAMx) and a particle trajectory model (FLEXPART) are used to evaluate the estimates of CO and SO2 in the current emission inventory using mesoscale meteorological simulations from MM5. Vertical column measurements of CO are used to constrain the total amount of emitted CO in the model and to identify the most appropriate vertical dispersion scheme. Zenith sky UV spectroscopy is used to estimate the emissions of SO2 from a large power plant and the Popocatépetl volcano. Results suggest that the models are able to identify correctly large point sources and that both the power plant and the volcano impact the MCMA. Modelled concentrations of CO based on the current emission inventory match observations suggesting that the current total emissions estimate is correct. Possible adjustments to the spatial and temporal distribution can be inferred from model results. Accurate source and dispersion modelling provides feedback for development of the emission inventory, verification of transport processes in air quality models and guidance for policy decisions