scholarly journals Air quality and radiative forcing impacts of anthropogenic volatile organic compound emissions from ten world regions

2014 ◽  
Vol 14 (2) ◽  
pp. 523-535 ◽  
Author(s):  
M. M. Fry ◽  
M. D. Schwarzkopf ◽  
Z. Adelman ◽  
J. J. West
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Chemical Transport Model ◽  
Large Variability ◽  
Volatile Organic

Abstract. Non-methane volatile organic compounds (NMVOCs) influence air quality and global climate change through their effects on secondary air pollutants and climate forcers. Here we simulate the air quality and radiative forcing (RF) impacts of changes in ozone, methane, and sulfate from halving anthropogenic NMVOC emissions globally and from 10 regions individually, using a global chemical transport model and a standalone radiative transfer model. Halving global NMVOC emissions decreases global annual average tropospheric methane and ozone by 36.6 ppbv and 3.3 Tg, respectively, and surface ozone by 0.67 ppbv. All regional reductions slow the production of peroxyacetyl nitrate (PAN), resulting in regional to intercontinental PAN decreases and regional NOx increases. These NOx increases drive tropospheric ozone increases nearby or downwind of source regions in the Southern Hemisphere (South America, Southeast Asia, Africa, and Australia). Some regions' NMVOC emissions contribute importantly to air pollution in other regions, such as East Asia, the Middle East, and Europe, whose impact on US surface ozone is 43%, 34%, and 34% of North America's impact. Global and regional NMVOC reductions produce widespread negative net RFs (cooling) across both hemispheres from tropospheric ozone and methane decreases, and regional warming and cooling from changes in tropospheric ozone and sulfate (via several oxidation pathways). The 100 yr and 20 yr global warming potentials (GWP100, GWP20) are 2.36 and 5.83 for the global reduction, and 0.079 to 6.05 and −1.13 to 18.9 among the 10 regions. The NMVOC RF and GWP estimates are generally lower than previously modeled estimates, due to the greater NMVOC/NOx emissions ratios simulated, which result in less sensitivity to NMVOC emissions changes and smaller global O3 burden responses, in addition to differences in the representation of NMVOCs and oxidation chemistry among models. Accounting for a fuller set of RF contributions may change the relative magnitude of each region's impacts. The large variability in the RF and GWP of NMVOCs among regions suggest that regionally specific metrics may be necessary to include NMVOCs in multi-gas climate trading schemes.

scholarly journals Air quality and radiative forcing impacts of anthropogenic volatile organic compound emissions from ten world regions

2013 ◽  
Vol 13 (8) ◽  
pp. 21125-21157 ◽  
Author(s):  
M. M. Fry ◽  
M. D. Schwarzkopf ◽  
Z. Adelman ◽  
J. J. West
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Chemical Transport Model ◽  
Large Variability ◽  
Volatile Organic

Abstract. Non-methane volatile organic compounds (NMVOCs) influence air quality and global climate change through their effects on secondary air pollutants and climate forcers. Here we simulate the air quality and radiative forcing (RF) impacts of changes in ozone, methane, and sulfate from halving anthropogenic NMVOC emissions globally and from 10 regions individually, using a global chemical transport model and a standalone radiative transfer model. Halving global NMVOC emissions decreases global annual average tropospheric methane and ozone by 36.6 ppbv and 3.3 Tg, respectively, and surface ozone by 0.67 ppbv. All regional reductions slow the production of PAN, resulting in regional to intercontinental PAN decreases and regional NOx increases. These NOx increases drive tropospheric ozone increases nearby or downwind of source regions in the Southern Hemisphere (South America, Southeast Asia, Africa, and Australia). Some regions' NMVOC emissions contribute importantly to air pollution in other regions, such as East Asia, Middle East, and Europe, whose impact on US surface ozone is 43%, 34%, and 34% of North America's impact. Global and regional NMVOC reductions produce widespread negative net RFs (cooling) across both hemispheres from tropospheric ozone and methane decreases, and regional warming and cooling from changes in tropospheric ozone and sulfate (via several oxidation pathways). The total global net RF for NMVOCs is estimated as 0.0277 W m−2 (~1.8% of CO2 RF since the preindustrial). The 100 yr and 20 yr global warming potentials (GWP100, GWP20) are 2.36 and 5.83 for the global reduction, and 0.079 to 6.05 and −1.13 to 18.9 among the 10 regions. The NMVOC RF and GWP estimates are generally lower than previously modeled estimates, due to differences among models in ozone, methane, and sulfate sensitivities, and the climate forcings included in each estimate. Accounting for a~fuller set of RF contributions may change the relative magnitude of each region's impacts. The large variability in the RF and GWP of NMVOCs among regions suggest that regionally-specific metrics may be necessary to include NMVOCs in multi-gas climate trading schemes.

scholarly journals Net radiative forcing and air quality responses to regional CO emission reductions

2012 ◽  
Vol 12 (12) ◽  
pp. 33443-33488
Author(s):  
M. M. Fry ◽  
M. D. Schwarzkopf ◽  
Z. Adelman ◽  
V. Naik ◽  
W. J. Collins ◽  
...  
Keyword(s):  
Air Quality ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Ozone Production ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
International Climate Agreements ◽  
The Tropics ◽  
Reduction Region

Abstract. Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100-yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO yr−1)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO yr−1)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern mid-latitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.

scholarly journals Contrasting the direct radiative effect and direct radiative forcing of aerosols

2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  
Keyword(s):  
Energy Balance ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Radiative Effect ◽  
Chemical Transport Model ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Direct Radiative Forcing

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

scholarly journals Tropospheric ozone radiative forcing uncertainty due to pre-industrial fire and biogenic emissions

2020 ◽  
Vol 20 (18) ◽  
pp. 10937-10951
Author(s):  
Matthew J. Rowlinson ◽  
Alexandru Rap ◽  
Douglas S. Hamilton ◽  
Richard J. Pope ◽  
Stijn Hantson ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Biogenic Emissions ◽  
Transfer Model ◽  
Terrestrial Vegetation ◽  
Uncertainty Range ◽  
Ozone Concentrations ◽  
Industrial Fire

Abstract. Tropospheric ozone concentrations are sensitive to natural emissions of precursor compounds. In contrast to existing assumptions, recent evidence indicates that terrestrial vegetation emissions in the pre-industrial era were larger than in the present day. We use a chemical transport model and a radiative transfer model to show that revised inventories of pre-industrial fire and biogenic emissions lead to an increase in simulated pre-industrial ozone concentrations, decreasing the estimated pre-industrial to present-day tropospheric ozone radiative forcing by up to 34 % (0.38 to 0.25 W m−2). We find that this change is sensitive to employing biomass burning and biogenic emissions inventories based on matching vegetation patterns, as the co-location of emission sources enhances the effect on ozone formation. Our forcing estimates are at the lower end of existing uncertainty range estimates (0.2–0.6 W m−2), without accounting for other sources of uncertainty. Thus, future work should focus on reassessing the uncertainty range of tropospheric ozone radiative forcing.

scholarly journals Tropospheric bromine chemistry: implications for present and pre-industrial ozone and mercury

2012 ◽  
Vol 12 (15) ◽  
pp. 6723-6740 ◽  
Author(s):  
J. P. Parrella ◽  
D. J. Jacob ◽  
Q. Liang ◽  
Y. Zhang ◽  
L. J. Mickley ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Elemental Mercury ◽  
Tropospheric Chemistry ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Mixing Ratios ◽  
The North

Abstract. We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1–8 nmol mol−1 (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

scholarly journals Tropospheric bromine chemistry: implications for present and pre-industrial ozone and mercury

2012 ◽  
Vol 12 (4) ◽  
pp. 9665-9715 ◽  
Author(s):  
J. P. Parrella ◽  
D. J. Jacob ◽  
Q. Liang ◽  
Y. Zhang ◽  
L. J. Mickley ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Elemental Mercury ◽  
Tropospheric Chemistry ◽  
The Arctic ◽  
Chemical Transport Model ◽  
The North ◽  
Subsurface Waters

Abstract. We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone concentrations by <1−8 nmol mol−1 (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

scholarly journals Net radiative forcing and air quality responses to regional CO emission reductions

2013 ◽  
Vol 13 (10) ◽  
pp. 5381-5399 ◽  
Author(s):  
M. M. Fry ◽  
M. D. Schwarzkopf ◽  
Z. Adelman ◽  
V. Naik ◽  
W. J. Collins ◽  
...  
Keyword(s):  
Air Quality ◽  
Radiative Forcing ◽  
Surface Ozone ◽  
Ozone Production ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Geophysical Fluid Dynamics Laboratory ◽  
International Climate Agreements ◽  
The Tropics ◽  
Reduction Region

Abstract. Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL (Geophysical Fluid Dynamics Laboratory) standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100 yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern midlatitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.

scholarly journals Tropospheric ozone radiative forcing uncertainty due to pre-industrial fire and biogenic emissions

2020 ◽  
Author(s):  
Matthew J. Rowlinson ◽  
Alexandru Rap ◽  
Douglas S. Hamilton ◽  
Richard J. Pope ◽  
Stijn Hantson ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Biogenic Emissions ◽  
Transfer Model ◽  
Terrestrial Vegetation ◽  
Uncertainty Range ◽  
Ozone Concentrations ◽  
Industrial Fire

Abstract. Tropospheric ozone concentrations are sensitive to natural emissions of precursor compounds. In contrast to existing assumptions, recent evidence indicates that terrestrial vegetation emissions in the pre-industrial were larger than in the present-day. We use a chemical transport model and a radiative transfer model to show that revised inventories of pre-industrial fire and biogenic emissions lead to an increase in simulated pre-industrial ozone concentrations, decreasing the estimated pre-industrial to present-day tropospheric ozone radiative forcing of up to 34 % (0.38 W m-2 to 0.25 W m-2). We find that this change is sensitive to employing biomass burning and biogenic emissions inventories based on matching vegetation patterns, as co-location of emission sources enhances the effect on ozone formation. Our forcing estimates are at the lower end of existing uncertainty range estimates (0.2–0.6 W m-22), without accounting for other sources of uncertainty. Thus, future work should focus on reassessing the uncertainty range of tropospheric ozone radiative forcing.

scholarly journals Assessing Douro Vineyards Exposure to Tropospheric Ozone

Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 200
Author(s):  
Ana Ascenso ◽  
Carla Gama ◽  
Daniel Blanco-Ward ◽  
Alexandra Monteiro ◽  
Carlos Silveira ◽  
...  
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Sugar Content ◽  
Productivity Loss ◽  
Ozone Exposure ◽  
Vitis Vinifera L ◽  
Chemical Transport Model ◽  
Wine Production ◽  
Exposure Response

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.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

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.

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