scholarly journals Ozone response to emission changes: a modeling study during the MCMA-2006/MILAGRO Campaign

2010 ◽  
Vol 10 (8) ◽  
pp. 3827-3846 ◽  
Author(s):  
J. Song ◽  
W. Lei ◽  
N. Bei ◽  
M. Zavala ◽  
B. de Foy ◽  
...  

Abstract. The sensitivity of ozone production to precursor emissions was investigated under five different meteorological conditions in the Mexico City Metropolitan Area (MCMA) during the MCMA-2006/MILAGRO field campaign using the gridded photochemical model CAMx driven by observation-nudged WRF meteorology. Precursor emissions were constrained by the comprehensive data from the field campaign and the routine ambient air quality monitoring network. Simulated plume mixing and transport were examined by comparing with measurements from the G-1 aircraft during the campaign. The observed concentrations of ozone precursors and ozone were reasonably well reproduced by the model. The effects of reducing precursor emissions on urban ozone production were performed for three representative emission control scenarios. A 50% reduction in VOC emissions led to 7 to 22 ppb decrease in daily maximum ozone concentrations, while a 50% reduction in NOx emissions leads to 4 to 21 ppb increase, and 50% reductions in both NOx and VOC emission decrease the daily maximum ozone concentrations up to 10 ppb. These results along with a chemical indicator analysis using the chemical production ratios of H2O2 to HNO3 demonstrate that the MCMA urban core region is VOC-limited for all meteorological episodes, which is consistent with the results from MCMA-2003 field campaign; however the degree of the VOC-sensitivity is higher during MCMA-2006 due to lower VOCs, lower VOC reactivity and moderately higher NOx emissions. Ozone formation in the surrounding mountain/rural area is mostly NOx-limited, but can be VOC-limited, and the range of the NOx-limited or VOC-limited areas depends on meteorology.

2009 ◽  
Vol 9 (6) ◽  
pp. 23419-23463 ◽  
Author(s):  
J. Song ◽  
W. Lei ◽  
N. Bei ◽  
M. Zavala ◽  
B. de Foy ◽  
...  

Abstract. The sensitivity of ozone production to precursor emissions was investigated under five different meteorological conditions in the Mexico City Metropolitan Area (MCMA) during the MCMA-2006/MILAGRO field campaign using the gridded photochemical model CAMx driven by observation-nudged WRF meteorology. Precursor emissions were constrained by the comprehensive data from the field campaign and the routine ambient air quality monitoring network. Simulated plume mixing and transport were examined by comparing with measurements from the G-1 aircraft during the campaign. The observed concentrations of ozone precursors and ozone were well reproduced by the model. The effects of reducing precursor emissions on urban ozone production were performed for three representative emission control strategies. A 50% reduction in VOC emissions led to 7 to 22 ppb decrease in daily maximum ozone concentrations, while a 50% reduction in NOx emissions leads to 4 to 21 ppb increase, and 50% reductions in both NOx and VOC emission decrease the daily maximum ozone concentrations up to 10 ppb. These results along with a chemical indicator analysis using the chemical production ratios of H2O2 to HNO3 demonstrate that the MCMA urban core region is VOC-limited for all meteorological episodes, which is consistent with the results from MCMA-2003 field campaign; however the degree of the VOC-sensitivity is higher in the MCMA-2006 due to lower VOC/NOx emission ratio and VOC reactivity. Ozone formation in the surrounding mountain/rural area is mostly NOx-limited, but can be VOC-limited, and the range of the NOx-limited or VOC-limited areas depends on meteorology.


2012 ◽  
Vol 12 (16) ◽  
pp. 7399-7412 ◽  
Author(s):  
A. Zare ◽  
J. H. Christensen ◽  
P. Irannejad ◽  
J. Brandt

Abstract. Knowledge about isoprene emissions and concentration distribution is important for chemistry transport models (CTMs), because isoprene acts as a precursor for tropospheric ozone and subsequently affects the atmospheric concentrations of many other atmospheric compounds. Isoprene has a short lifetime, and hence it is very difficult to evaluate its emission estimates against measurements. For this reason, we coupled two isoprene emission models with the Danish Eulerian Hemispheric Model (DEHM), and evaluated the simulated background ozone concentrations based on different models for isoprene emissions. In this research, results of using the two global biogenic emission models; GEIA (Global Emissions Inventory Activity) and MEGAN (the global Model of Emissions of Gases and Aerosols from Nature) are compared and evaluated. The total annual emissions of isoprene for the year 2006 estimated by using MEGAN is 592 Tg yr−1 for an extended area of the Northern Hemisphere, which is 21% higher than that estimated by using GEIA. The overall feature of the emissions from the two models is quite similar, but differences are found mainly in Africa's savannah and in the southern part of North America. Differences in spatial distribution of emission factors are found to be a key source of these discrepancies. In spite of the short life-time of isoprene, a direct evaluation of isoprene concentrations using the two biogenic emission models in DEHM has been made against available measurements in Europe. Results show an agreement between two models simulations and the measurements in general and that the CTM is able to simulate isoprene concentrations. Additionally, investigation of ozone concentrations resulting from the two biogenic emission models show that isoprene simulated by MEGAN strongly affects the ozone production in the African savannah; the effect is up to 10% more than that obtained using GEIA. In contrast, the impact of using GEIA is higher in the Amazon region with more than 8% higher ozone concentrations compared to that of using MEGAN. Comparing the ozone concentrations obtained by DEHM using the two different isoprene models with measurements from Europe and North America, show an agreement on the hourly, mean daily and daily maximum values. However, the average of ozone daily maximum value simulated by using MEGAN is slightly closer to the measured value for the average of all measuring sites in Europe.


2017 ◽  
Author(s):  
Paul S. Romer ◽  
Kaitlin C. Duffey ◽  
Paul J. Wooldridge ◽  
Eric Edgerton ◽  
Karsten Baumann ◽  
...  

Abstract. Surface ozone concentrations are observed to increase with rising temperatures, but the mechanisms responsible for this effect in rural and remote continental regions remain uncertain. Better understanding of the effects of temperature on ozone is crucial to understanding global air quality and how it may be affected by climate change. We combine measurements from a focused ground campaign in summer 2013 with a long-term record from a forested site in the rural southeast United States to examine how daily average temperature affects ozone production. We find that changes to local chemistry are key drivers of increased ozone concentrations on hotter days, with integrated daily ozone production increasing by 2.3 ppb C−1. Nearly half of this increase is attributable to temperature-driven increases in emissions of nitrogen oxides (NOx), most likely by soil microbes. The increase of soil NOx emissions with temperature suggests that ozone will continue to increase with temperature in the future, even as direct anthropogenic NOx emissions decrease dramatically. The links between temperature, soil NOx, and ozone form a positive climate feedback.


2018 ◽  
Vol 18 (4) ◽  
pp. 2601-2614 ◽  
Author(s):  
Paul S. Romer ◽  
Kaitlin C. Duffey ◽  
Paul J. Wooldridge ◽  
Eric Edgerton ◽  
Karsten Baumann ◽  
...  

Abstract. Surface ozone concentrations are observed to increase with rising temperatures, but the mechanisms responsible for this effect in rural and remote continental regions remain uncertain. Better understanding of the effects of temperature on ozone is crucial to understanding global air quality and how it may be affected by climate change. We combine measurements from a focused ground campaign in summer 2013 with a long-term record from a forested site in the rural southeastern United States, to examine how daily average temperature affects ozone production. We find that changes to local chemistry are key drivers of increased ozone concentrations on hotter days, with integrated daily ozone production increasing by 2.3 ppb ∘C−1. Nearly half of this increase is attributable to temperature-driven increases in emissions of nitrogen oxides (NOx), most likely by soil microbes. The increase of soil NOx emissions with temperature suggests that ozone will continue to increase with temperature in the future, even as direct anthropogenic NOx emissions decrease dramatically. The links between temperature, soil NOx, and ozone form a positive climate feedback.


2012 ◽  
Vol 12 (5) ◽  
pp. 2567-2585 ◽  
Author(s):  
Y. Kanaya ◽  
A. Hofzumahaus ◽  
H.-P. Dorn ◽  
T. Brauers ◽  
H. Fuchs ◽  
...  

Abstract. A photochemical box model constrained by ancillary observations was used to simulate OH and HO2 concentrations for three days of ambient observations during the HOxComp field campaign held in Jülich, Germany in July 2005. Daytime OH levels observed by four instruments were fairly well reproduced to within 33% by a base model run (Regional Atmospheric Chemistry Mechanism with updated isoprene chemistry adapted from Master Chemical Mechanism ver. 3.1) with high R2 values (0.72–0.97) over a range of isoprene (0.3–2 ppb) and NO (0.1–10 ppb) mixing ratios. Daytime HO2(*) levels, reconstructed from the base model results taking into account the sensitivity toward speciated RO2 (organic peroxy) radicals, as recently reported from one of the participating instruments in the HO2 measurement mode, were 93% higher than the observations made by the single instrument. This also indicates an overprediction of the HO2 to OH recycling. Together with the good model-measurement agreement for OH, it implies a missing OH source in the model. Modeled OH and HO2(*) could only be matched to the observations by addition of a strong unknown loss process for HO2(*) that recycles OH at a high yield. Adding to the base model, instead, the recently proposed isomerization mechanism of isoprene peroxy radicals (Peeters and Müller, 2010) increased OH and HO2(*) by 28% and 13% on average. Although these were still only 4% higher than the OH observations made by one of the instruments, larger overestimations (42–70%) occurred with respect to the OH observations made by the other three instruments. The overestimation in OH could be diminished only when reactive alkanes (HC8) were solely introduced to the model to explain the missing fraction of observed OH reactivity. Moreover, the overprediction of HO2(*) became even larger than in the base case. These analyses imply that the rates of the isomerization are not readily supported by the ensemble of radical observations. One of the measurement days was characterized by low isoprene concentrations (∼0.5 ppb) and OH reactivity that was well explained by the observed species, especially before noon. For this selected period, as opposed to the general behavior, the model tended to underestimate HO2(*). We found that this tendency is associated with high NOx concentrations, suggesting that some HO2 production or regeneration processes under high NOx conditions were being overlooked; this might require revision of ozone production regimes.


2021 ◽  
pp. 118624
Author(s):  
Fangzhou Guo ◽  
Alexander A.T. Bui ◽  
Benjamin C. Schulze ◽  
Subin Yoon ◽  
Sujan Shrestha ◽  
...  

1987 ◽  
Vol 21 (12) ◽  
pp. 2673-2679 ◽  
Author(s):  
Fouad I. Kanbour ◽  
Shatha Y. Faiq ◽  
Faiza A. Al-Taie ◽  
Abdul Messih N. Kitto ◽  
Nessren Bader

2016 ◽  
Vol 217 ◽  
pp. 42-51 ◽  
Author(s):  
Carola Graf ◽  
Athanasios Katsoyiannis ◽  
Kevin C. Jones ◽  
Andrew J. Sweetman

2010 ◽  
Vol 3 (4) ◽  
pp. 2291-2314
Author(s):  
G. Sarwar ◽  
K. W. Appel ◽  
A. G. Carlton ◽  
R. Mathur ◽  
K. Schere ◽  
...  

Abstract. A new condensed toluene mechanism is incorporated into the Community Multiscale Air Quality Modeling system. Model simulations are performed using the CB05 chemical mechanism containing the existing (base) and the new toluene mechanism for the western and eastern US for a summer month. With current estimates of tropospheric emission burden, the new toluene mechanism increases monthly mean daily maximum 8-h ozone by 1.0–3.0 ppbv in Los Angeles, Portland, Seattle, Chicago, Cleveland, northeastern US, and Detroit compared to that with the base toluene chemistry. It reduces model mean bias for ozone at elevated observed ozone mixing ratios. While the new mechanism increases predicted ozone, it does not enhance ozone production efficiency. Sensitivity study suggests that it can further enhance ozone if elevated toluene emissions are present. While changes in total fine particulate mass are small, predictions of in-cloud SOA increase substantially.


2016 ◽  
Vol 16 (18) ◽  
pp. 11601-11615 ◽  
Author(s):  
Jane Coates ◽  
Kathleen A. Mar ◽  
Narendra Ojha ◽  
Tim M. Butler

Abstract. Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NOx). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NOx and temperature, and we compared this to previous observational studies. Under high-NOx conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NOx emissions. CB05 and RADM2 simulated more NOx-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of Ox production; the net influence of peroxy nitrates increased net Ox production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NOx emissions would be required to offset the additional ozone production due to an increase in temperature in the future.


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