scholarly journals Photochemical environment over Southeast Asia primed for hazardous ozone levels with influx of nitrogen oxides from seasonal biomass burning

2020 ◽  
Author(s):  
Margaret R. Marvin ◽  
Paul I. Palmer ◽  
Barry G. Latter ◽  
Richard Siddans ◽  
Brian J. Kerridge ◽  
...  

Abstract. Mainland and maritime Southeast Asia are home to more than 655 million people, representing nearly 10 % of the global population. The dry season in this region is typically associated with intense biomass burning activity, which leads to a significant increase in surface air pollutants that are harmful to human health, including ozone (O3). Latitude-based differences in dry season and land use distinguish two regional biomass burning regimes: (1) burning on the peninsular mainland peaking in March and (2) burning across Indonesia peaking in September. The type and amount of material burned in each regime impacts the emissions of nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs), which combine to produce ozone. Here, we use the nested GEOS-Chem atmospheric chemistry transport model (horizontal resolution of 0.25° × 0.3125°), in combination with satellite observations from the Ozone Monitoring Instrument (OMI) and ground-based observations from Malaysia, to investigate ozone photochemistry over Southeast Asia in 2014. Seasonal cycles of tropospheric ozone columns from OMI and GEOS-Chem peak with biomass burning emissions. Compared to OMI, the model has a mean annual bias of −11 % but tends to overestimate tropospheric ozone near areas of seasonal fire activity. We find that outside of these burning areas, the underlying photochemical environment is generally NOx-limited, dominated by anthropogenic NOx and biogenic non-methane VOC emissions. Pyrogenic emissions of NOx play a key role in photochemistry, shifting towards more VOC-limited ozone production and contributing about 30 % of the regional ozone formation potential during both biomass burning seasons. Using the GEOS-Chem model, we find that biomass burning activity coincides with widespread ozone exposure at levels that exceed world public health guidelines, resulting in 272 premature deaths on mainland Southeast Asia in March of 2014 and another 273 deaths across Indonesia in September. Despite a positive model bias, hazardous ozone levels are confirmed by surface observations during both burning seasons.

2021 ◽  
Vol 21 (3) ◽  
pp. 1917-1935
Author(s):  
Margaret R. Marvin ◽  
Paul I. Palmer ◽  
Barry G. Latter ◽  
Richard Siddans ◽  
Brian J. Kerridge ◽  
...  

Abstract. Mainland and maritime Southeast Asia is home to more than 655 million people, representing nearly 10 % of the global population. The dry season in this region is typically associated with intense biomass burning activity, which leads to a significant increase in surface air pollutants that are harmful to human health, including ozone (O3). Latitude-based differences in the dry season and land use distinguish two regional biomass burning regimes: (1) burning on the peninsular mainland peaking in March and (2) burning across Indonesia peaking in September. The type and amount of material burned in each regime impact the emissions of nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs), which combine to produce ozone. Here, we use the nested GEOS-Chem atmospheric chemistry transport model (horizontal resolution of 0.25∘ × 0.3125∘), in combination with satellite observations from the Ozone Monitoring Instrument (OMI) and ground-based observations from Malaysia, to investigate ozone photochemistry over Southeast Asia in 2014. Seasonal cycles of tropospheric ozone columns from OMI and GEOS-Chem peak with biomass burning emissions. Compared to OMI, the model has a mean annual bias of −11 % but tends to overestimate tropospheric ozone near areas of seasonal fire activity. We find that outside these burning areas, the underlying photochemical environment is generally NOx-limited and dominated by anthropogenic NOx and biogenic non-methane VOC emissions. Pyrogenic emissions of NOx play a key role in photochemistry, shifting towards more VOC-limited ozone production and contributing about 30 % of the regional ozone formation potential during both biomass burning seasons. Using the GEOS-Chem model, we find that biomass burning activity coincides with widespread ozone exposure at levels that exceed world public health guidelines, resulting in about 260 premature deaths across Southeast Asia in March 2014 and another 160 deaths in September. Despite a positive model bias, hazardous ozone levels are confirmed by surface observations during both burning seasons.


2020 ◽  
Author(s):  
Margaret Marvin ◽  
Paul Palmer ◽  
Fei Yao ◽  
Barry Latter ◽  
Richard Siddans ◽  
...  

<p>Mainland and maritime Southeast Asia is home to more than 655 million people, representing nearly 10% of the global population. The dry season in this region is typically associated with intense biomass burning activity, which leads to a significant increase in surface air pollutants that are harmful to human health, including ozone (O<sub>3</sub>) and fine (radii smaller than 2.5 microns) particulate matter (PM<sub>2.5</sub>). Latitude-based differences in dry season timing and land use distinguish two regional biomass burning regimes: (1) agricultural waste burning on the peninsular mainland from February through April and (2) coastal peat burning across the equatorial islands in September and October. The type and amount of material burned determines the chemical composition of emissions and subsequently their impact on regional air quality. Understanding the individual and collective roles of these biomass burning regimes is a crucial step towards developing effective air quality mitigation strategies for Southeast Asia. Here, we use the nested GEOS-Chem atmospheric chemistry transport model (horizontal resolution of 0.25° x 0.3125°) to simulate fire-atmosphere interactions over Southeast Asia during March and September of 2014, when emissions peak from the two regional burning seasons. Based on our analysis of model output, we report how these two distinct biomass burning regimes impact the photochemical environment over Southeast Asia and what the resulting consequences are for surface air quality. We will also present a critical evaluation of our model using ground-based and satellite observations of atmospheric composition across the region.</p>


2014 ◽  
Vol 14 (17) ◽  
pp. 24573-24621 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  

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.


2015 ◽  
Vol 15 (11) ◽  
pp. 6047-6068 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 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, ΔO3/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 (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in 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 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 HOx 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.


Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 200
Author(s):  
Ana Ascenso ◽  
Carla Gama ◽  
Daniel Blanco-Ward ◽  
Alexandra Monteiro ◽  
Carlos Silveira ◽  
...  

Tropospheric ozone (O3) can strongly damage vegetation. Grapevines (Vitis vinifera L.), in particular, have intermediate sensitivity to ozone. Wine production is an important economic activity, as well as a pillar to the cultural identity of several countries in the world. This study aims to evaluate the risk of Douro vineyards exposure to ozone, by estimating its concentration and deposition in the Demarcated Region of Douro in Portugal. Based on an assessment of the climatology of the area, the years 2003 to 2005 were selected among the hottest years of the recent past, and the chemical transport model CHIMERE was used to estimate the three-dimensional field of ozone and its dry deposition over the Douro region with 1 km2 of horizontal resolution. Model results were validated by comparison with measured data from the European air quality database (AirBase). The exposure indicator AOT40 (accumulated concentration of ozone above 40 ppb) was calculated and an exposure–response function was applied to determine the grapevine risk to ozone exposure. The target value for the protection of vegetation established by the Air Quality Framework Directive was exceeded on most of the Douro region, especially over the Baixo Corgo and Cima Corgo sub-regions. The results of the exposure–response functions suggest that the productivity loss can reach 27% and that the sugar content of the grapes could be reduced by 32%, but these values are affected by the inherent uncertainty of the used methodology.


2016 ◽  
Author(s):  
Gerard Ancellet ◽  
Nikos Daskalakis ◽  
Jean Christophe Raut ◽  
Boris Quennehen ◽  
François Ravetta ◽  
...  

Abstract. The goal of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6–15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0–4 km and 4–8 km. For Canada, the model CO distribution and the weak correlation (< 30 %) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation (> 40 %) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient −6 to −8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65° N, while STE contribution is more homogeneous in the latitude range 55° N to 70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77° N).


2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.


2017 ◽  
Author(s):  
Peter M. Edwards ◽  
Mathew J. Evans

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.


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