scholarly journals Impact of Mexico City emissions on regional air quality from MOZART-4 simulations

2010 ◽  
Vol 10 (2) ◽  
pp. 3457-3498 ◽  
Author(s):  
L. K. Emmons ◽  
E. C. Apel ◽  
J.-F. Lamarque ◽  
P. G. Hess ◽  
M. Avery ◽  
...  
Keyword(s):  
Air Quality ◽  
Mexico City ◽  
Production Efficiency ◽  
Transport Model ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Model Calculations ◽  
Fire Emissions ◽  
Regional Air Quality

Abstract. An extensive set of measurements was made in and around Mexico City as part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) experiments in March 2006. Simulations with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4), a global chemical transport model, have been used to provide a regional context for these observations and assist in their interpretation. These MOZART-4 simulations reproduce the aircraft observations generally well, but some differences in the modeled volatile organic compounds (VOCs) from the observations result from incorrect VOC speciation assumed for the emission inventories. The different types of CO sources represented in the model have been "tagged" to quantify the contributions of regions outside Mexico, as well as the various emissions sectors within Mexico, to the regional air quality of Mexico. This analysis indicates open fires have some, but not a dominant, impact on the atmospheric composition in the region around Mexico City, when averaged over the month. However, considerable variation in the fire contribution (2–15% of total CO) is seen during the month. The transport and photochemical aging of Mexico City emissions were studied using tags of CO emissions for each day, showing that typically the air near Mexico City was a combination of many ages. Ozone production in MOZART-4 is shown to agree well with the net production rates from box model calculations constrained by the MILAGRO aircraft measurements. Ozone production efficiency derived from the ratio of Ox to NOz is higher in MOZART-4 than in the observations for moderately polluted air. OH reactivity determined from the MOZART-4 results shows the same increase in relative importance of oxygenated VOCs downwind of Mexico City as the reactivity inferred from the observations. The amount of ozone produced by emissions from Mexico City and surrounding areas has been quantified in the model by tracking NO emissions, showing little influence beyond Mexico's borders, and also relatively minor influence from fire emissions on the monthly average tropospheric ozone column.

scholarly journals Impact of Mexico City emissions on regional air quality from MOZART-4 simulations

2010 ◽  
Vol 10 (13) ◽  
pp. 6195-6212 ◽  
Author(s):  
L. K. Emmons ◽  
E. C. Apel ◽  
J.-F. Lamarque ◽  
P. G. Hess ◽  
M. Avery ◽  
...  
Keyword(s):  
Air Quality ◽  
Mexico City ◽  
Production Efficiency ◽  
Transport Model ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Model Calculations ◽  
Fire Emissions ◽  
Regional Air Quality

Abstract. An extensive set of measurements was made in and around Mexico City as part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) experiments in March 2006. Simulations with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4), a global chemical transport model, have been used to provide a regional context for these observations and assist in their interpretation. These MOZART-4 simulations reproduce the aircraft observations generally well, but some differences in the modeled volatile organic compounds (VOCs) from the observations result from incorrect VOC speciation assumed for the emission inventories. The different types of CO sources represented in the model have been "tagged" to quantify the contributions of regions outside Mexico, as well as the various emissions sectors within Mexico, to the regional air quality of Mexico. This analysis indicates open fires have some, but not a dominant, impact on the atmospheric composition in the region around Mexico City when averaged over the month. However, considerable variation in the fire contribution (2–15% of total CO) is seen during the month. The transport and photochemical aging of Mexico City emissions were studied using tags of CO emissions for each day, showing that typically the air downwind of Mexico City was a combination of many ages. Ozone production in MOZART-4 is shown to agree well with the net production rates from box model calculations constrained by the MILAGRO aircraft measurements. Ozone production efficiency derived from the ratio of Ox to NOz is higher in MOZART-4 than in the observations for moderately polluted air. OH reactivity determined from the MOZART-4 results shows the same increase in relative importance of oxygenated VOCs downwind of Mexico City as the reactivity inferred from the observations. The amount of ozone produced by emissions from Mexico City and surrounding areas has been quantified in the model by tracking NO emissions, showing little influence beyond Mexico's borders, and also relatively minor influence from fire emissions on the monthly average tropospheric ozone column.

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

2006 ◽  
Vol 6 (4) ◽  
pp. 7959-8009
Author(s):  
W. Lei ◽  
B. de Foy ◽  
M. Zavala ◽  
R. Volkamer ◽  
L. T. Molina
Keyword(s):  
Mexico City ◽  
Metropolitan Area ◽  
Production Efficiency ◽  
Transport Model ◽  
Ozone Production ◽  
Urban Region ◽  
Air Quality Model ◽  
Chemical Transport Model ◽  
Quality Model ◽  
Photochemical Production

Abstract. An 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/NOy<0.3) is VOC-limited. Both the simulated behavior of O3 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.

scholarly journals Effects of biogenic nitrate chemistry on the NO<sub>x</sub> lifetime in remote continental regions

2012 ◽  
Vol 12 (24) ◽  
pp. 11917-11932 ◽  
Author(s):  
E. C. Browne ◽  
R. C. Cohen
Keyword(s):  
Steady State ◽  
Air Quality ◽  
Production Efficiency ◽  
Transport Model ◽  
Ozone Production ◽  
Organic Nitrate ◽  
Chemical Transport Model ◽  
Global Budgets ◽  
Steady State Model ◽  
Order Of Magnitude

Abstract. We present an analysis of the NOx budget in conditions of low NOx (NOx = NO + NO2) and high biogenic volatile organic compound (BVOC) concentrations that are characteristic of most continental boundary layers. Using a steady-state model, we show that below 500 pptv of NOx, the NOx lifetime is extremely sensitive to organic nitrate (RONO2) formation rates. We find that even for RONO2 formation values that are an order of magnitude smaller than is typical for continental conditions significant reductions in NOx lifetime, and consequently ozone production efficiency, are caused by nitrate forming reactions. Comparison of the steady-state box model to a 3-D chemical transport model (CTM) confirms that the concepts illustrated by the simpler model are a useful approximation of predictions provided by the full CTM. This implies that the regional and global budgets of NOx, OH, and ozone will be sensitive to assumptions regarding organic nitrate chemistry. Changes in the budgets of these species affect the representation of processes important to air quality and climate. Consequently, CTMs must include an accurate representation of organic nitrate chemistry in order to provide accurate assessments of past, present, and future air quality and climate. These findings suggest the need for further experimental constraints on the formation and fate of biogenic RONO2.

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

2007 ◽  
Vol 7 (5) ◽  
pp. 1347-1366 ◽  
Author(s):  
W. Lei ◽  
B. de Foy ◽  
M. Zavala ◽  
R. Volkamer ◽  
L. T. Molina
Keyword(s):  
Mexico City ◽  
Metropolitan Area ◽  
Production Efficiency ◽  
Transport Model ◽  
Ozone Production ◽  
Urban Region ◽  
Air Quality Model ◽  
Chemical Transport Model ◽  
Quality Model ◽  
Photochemical Production

Abstract. An episodic simulation is conducted to characterize midday (12:00–17:00 CDT) ozone (O3) photochemical production and to investigate its sensitivity to emission changes of ozone precursors in the Mexico City Metropolitan Area (MCMA) during an "O3-South" meteorological episode 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/NOy<0.3) is VOC-limited. Both the simulated behavior of O3 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 estimates, and current NOx levels depress the O3 production.

scholarly journals Assessing the regional impacts of Mexico City emissions on air quality and chemistry

2009 ◽  
Vol 9 (11) ◽  
pp. 3731-3743 ◽  
Author(s):  
M. Mena-Carrasco ◽  
G. R. Carmichael ◽  
J. E. Campbell ◽  
D. Zimmerman ◽  
Y. Tang ◽  
...  
Keyword(s):  
Air Quality ◽  
Mexico City ◽  
Ozone Production ◽  
Anthropogenic Aerosol ◽  
Near Surface ◽  
Mixing Ratios ◽  
Regional Impacts ◽  
Photolysis Rates ◽  
Regional Air Quality ◽  
The Impact

Abstract. The impact of Mexico City (MCMA) emissions is examined by studying its effects on air quality, photochemistry, and on ozone production regimes by combining model products and aircraft observations from the MILAGRO experiment during March 2006. The modeled influence of MCMA emissions to enhancements in surface level NOx, CO, and O3 concentrations (10–30% increase) are confined to distances <200 km, near surface. However, the extent of the influence is significantly larger at higher altitudes. Broader MCMA impacts (some 900 km Northeast of the city) are shown for specific outflow conditions in which enhanced ozone, NOy, and MTBE mixing ratios over the Gulf of Mexico are linked to MCMA by source tagged tracers and sensitivity runs. This study shows that the "footprint" of MCMA on average is fairly local, with exception to reactive nitrogen, which can be transported long range in the form of PAN, acting as a reservoir and source of NOx with important regional ozone formation implications. The simulated effect of MCMA emissions of anthropogenic aerosol on photochemistry showed a maximum regional decrease of 40% in J[NO2→NO+O], and resulting in the reduction of ozone production by 5–10%. Observed ozone production efficiencies are evaluated as a function of distance from MCMA, and by modeled influence from MCMA. These tend to be much lower closer to MCMA, or in those points where modeled contribution from MCMA is large. This research shows that MCMA emissions do effect on regional air quality and photochemistry, both contributing large amounts of ozone and its precursors, but with caveat that aerosol concentrations hinder formation of ozone to its potential due to its reduction in photolysis rates.

scholarly journals A new diagnostic for tropospheric ozone production

2017 ◽  
Author(s):  
Peter M. Edwards ◽  
Mathew J. Evans
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
Chemical Transport Model ◽  
Organic Species ◽  
Earth’S Climate ◽  
Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

scholarly journals Pollution transport from North America to Greenland during summer 2008

2013 ◽  
Vol 13 (7) ◽  
pp. 3825-3848 ◽  
Author(s):  
J. L. Thomas ◽  
J.-C. Raut ◽  
K. S. Law ◽  
L. Marelle ◽  
G. Ancellet ◽  
...  
Keyword(s):  
North America ◽  
Transport Model ◽  
Ozone Production ◽  
The Arctic ◽  
Pollution Transport ◽  
Chemical Transport Model ◽  
Fire Emissions ◽  
Fire Plumes ◽  
Ozone Levels ◽  
Pollution Plumes

Abstract. Ozone pollution transported to the Arctic is a significant concern because of the rapid, enhanced warming in high northern latitudes, which is caused, in part, by short-lived climate forcers, such as ozone. Long-range transport of pollution contributes to background and episodic ozone levels in the Arctic. However, the extent to which plumes are photochemically active during transport, particularly during the summer, is still uncertain. In this study, regional chemical transport model simulations are used to examine photochemical production of ozone in air masses originating from boreal fire and anthropogenic emissions over North America and during their transport toward the Arctic during early July 2008. Model results are evaluated using POLARCAT aircraft data collected over boreal fire source regions in Canada (ARCTAS-B) and several days downwind over Greenland (POLARCAT-France and POLARCAT-GRACE). Model results are generally in good agreement with the observations, except for certain trace gas species over boreal fire regions, in some cases indicating that the fire emissions are too low. Anthropogenic and biomass burning pollution (BB) from North America was rapidly uplifted during transport east and north to Greenland where pollution plumes were observed in the mid- and upper troposphere during POLARCAT. A model sensitivity study shows that CO levels are in better agreement with POLARCAT measurements (fresh and aged fire plumes) upon doubling CO emissions from fires. Analysis of model results, using ΔO3/ΔCO enhancement ratios, shows that pollution plumes formed ozone during transport towards the Arctic. Fresh anthropogenic plumes have average ΔO3/ΔCO enhancement ratios of 0.63 increasing to 0.92 for aged anthropogenic plumes, indicating additional ozone production during aging. Fresh fire plumes are only slightly enhanced in ozone (ΔO3/ΔCO=0.08), but form ozone downwind with ΔO3/ΔCO of 0.49 for aged BB plumes (model-based run). We estimate that aged anthropogenic and BB pollution together made an important contribution to ozone levels with an average contribution for latitudes >55° N of up to 6.5 ppbv (18%) from anthropogenic pollution and 3 ppbv (5.2%) from fire pollution in the model domain in summer 2008.

scholarly journals Biomass burning influence on high latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

2014 ◽  
Vol 14 (17) ◽  
pp. 24573-24621 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  
Keyword(s):  
Biomass Burning ◽  
High Latitude ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
The Arctic ◽  
Vertical Position ◽  
Chemical Transport Model ◽  
Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high laititudes (> 50˚ N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, Δ O3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.44–6.28 pptv ppbv−1) than GEOS5-forced models (2.02–3.02 pptv ppbv−1), which we show is likely linked to differences efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from Asia towards the Arctic using a Lagrangian chemical transport model show that 4 day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HO2 from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high latitude tropospheric ozone during summer.

scholarly journals The Meteorology-Chemistry Interface Processor (MCIP) for the CMAQ modeling system

2009 ◽  
Vol 2 (2) ◽  
pp. 1449-1486 ◽  
Author(s):  
T. L. Otte ◽  
J. E. Pleim
Keyword(s):  
Air Quality ◽  
Environmental Protection Agency ◽  
Transport Model ◽  
Control Strategies ◽  
Global Climate ◽  
Environmental Modeling ◽  
Chemical Transport Model ◽  
Meteorological Model ◽  
Vertical Coordinate ◽  
Regional Air Quality

Abstract. The Community Multiscale Air Quality (CMAQ) modeling system, a state-of-the-science regional air quality modeling system developed by the US Environmental Protection Agency, is being used for a variety of environmental modeling problems including regulatory applications, air quality forecasting, evaluation of emissions control strategies, process-level research, and interactions of global climate change and regional air quality. The Meteorology-Chemistry Interface Processor (MCIP) is a vital piece of software within the CMAQ modeling system that serves to, as best as possible, maintain dynamic consistency between the meteorological model and the chemical transport model. MCIP acts as both a post-processor to the meteorological model and a pre-processor to the CMAQ modeling system. MCIP's functions are to ingest the meteorological model output fields in their native formats, perform horizontal and vertical coordinate transformations, diagnose additional atmospheric fields, define gridding parameters, and prepare the meteorological fields in a form required by the CMAQ modeling system. This paper provides an updated overview of MCIP, documenting the scientific changes that have been made since it was first released as part of the CMAQ modeling system in 1998.

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

2008 ◽  
Vol 8 (24) ◽  
pp. 7571-7581 ◽  
Author(s):  
W. Lei ◽  
M. Zavala ◽  
B. de Foy ◽  
R. Volkamer ◽  
L. T. Molina
Keyword(s):  
Mexico City ◽  
Transport Model ◽  
Source Area ◽  
Meteorological Conditions ◽  
Pollutant Emissions ◽  
Ozone Production ◽  
Emissions Reduction ◽  
Chemical Transport Model ◽  
Transport Pathway ◽  
Chemical Aging

Abstract. Photochemistry in polluted atmospheres, 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 emissions reduction under three distinctively different meteorological conditions in the Mexico City Metropolitan Area during the MCMA-2003 field measurement campaign. The O3 formation characteristics and sensitivity to emissions change were found to be weakly dependent on the meteorological conditions. The evolution of O3 formation and its sensitivity to NOx and VOC levels 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 downwind plumes were characterized with low and constant O3 production, and plumes along their transport pathway were characterized 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.

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