Biogenic Hydrocarbon Emissions Research Articles

Segregation of Fast-Reactive Species in Atmospheric Turbulent Flow

Atmospheric turbulence, which produces chaotic motions in the planetary boundary layer, can inhibit mixing between fast-reacting species produced or released at different locations. This segregation process modifies the effective rate at which reactions occur between these species and is not appropriately accounted for in coarse-resolution models, since these models assume complete mixing of tracers within each grid box. Here, we present a few examples of large-eddy simulations (LES) applied to chemically reactive species in a forested area with high emissions of biogenic hydrocarbons, an urban area rich in anthropogenic emissions, and a maritime area with high emissions of reduced sulfur species.

Comprehensive isoprene and terpene gas-phase chemistry improves simulated surface ozone in the southeastern US

Abstract. Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Past studies have suggested different solutions including the need for updates to model representation of clouds, chemistry, ozone deposition, and emissions of nitrogen oxides (NOx) or biogenic hydrocarbons. Here, due to the high biogenic emissions in the southeastern US, more comprehensive and updated isoprene and terpene chemistry is added into CESM/CAM-chem (Community Earth System Model/Community Atmosphere Model with full chemistry) to evaluate the impact of chemistry on simulated ozone. Comparisons of the model results with data collected during the Studies of Emissions Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign and from the US EPA (Environmental Protection Agency) CASTNET (Clean Air Status and Trends Network) monitoring stations confirm the updated chemistry improves simulated surface ozone, ozone precursors, and NOx reservoir compounds. The isoprene and terpene chemistry updates reduce the bias in the daily maximum 8 h average (MDA8) surface ozone by up to 7 ppb. In the past, terpene oxidation in particular has been ignored or heavily reduced in chemical schemes used in many regional and global models, and this study demonstrates that comprehensive isoprene and terpene chemistry is needed to reduce surface ozone model biases. Sensitivity tests were performed in order to evaluate the impact of lingering uncertainties in isoprene and terpene oxidation on ozone. Results suggest that even though isoprene emissions are higher than terpene emissions in the southeastern US, remaining uncertainties in isoprene and terpene oxidation have similar impacts on ozone due to lower uncertainties in isoprene oxidation. Additionally, this study identifies the need for further constraints on the aerosol uptake of organic nitrates derived from isoprene and terpenes in order to reduce uncertainty in simulated ozone. Although the updates to isoprene and terpene chemistry greatly reduce the ozone bias in CAM-chem, a large bias remains. Evaluation against SEAC4RS field campaign results suggests future improvements to horizontal resolution and cloud parameterizations in CAM-chem may be particularly important for further reducing this bias.

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

AbstractDuring an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NOx) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NOx. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NOx concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NOx (NO < 0.08 and NO2 < 0.46 ppbv) and high biogenic hydrocarbon emissions.

Biogenic hydrocarbon emissions: a consideration for large-scale tree planting programs

Biogenic hydrocarbon emissions: a consideration for large-scale tree planting programs

Modeling the Current and Future Roles of Particulate Organic Nitrates in the Southeastern United States.

Organic nitrates are an important aerosol constituent in locations where biogenic hydrocarbon emissions mix with anthropogenic NOx sources. While regional and global chemical transport models may include a representation of organic aerosol from monoterpene reactions with nitrate radicals (the primary source of particle-phase organic nitrates in the Southeast United States), secondary organic aerosol (SOA) models can underestimate yields. Furthermore, SOA parametrizations do not explicitly take into account organic nitrate compounds produced in the gas phase. In this work, we developed a coupled gas and aerosol system to describe the formation and subsequent aerosol-phase partitioning of organic nitrates from isoprene and monoterpenes with a focus on the Southeast United States. The concentrations of organic aerosol and gas-phase organic nitrates were improved when particulate organic nitrates were assumed to undergo rapid (τ = 3 h) pseudohydrolysis resulting in nitric acid and nonvolatile secondary organic aerosol. In addition, up to 60% of less oxidized-oxygenated organic aerosol (LO-OOA) could be accounted for via organic nitrate mediated chemistry during the Southern Oxidants and Aerosol Study (SOAS). A 25% reduction in nitrogen oxide (NO + NO2) emissions was predicted to cause a 9% reduction in organic aerosol for June 2013 SOAS conditions at Centreville, Alabama.

Impact of regional transport on the anthropogenic and biogenic secondary organic aerosols in the Los Angeles Basin

This manuscript explores the role of regional transport on anthropogenic and biogenic secondary organic carbon (SOC) concentrations in ambient fine particulate (PM2.5) organic carbon (OC) in the Los Angeles (LA) Basin. Daily organic molecular markers, water soluble organic carbon (WSOC), OC, and elemental carbon (EC) measurements from May 2009 through April 2010 at a central site in downtown LA, and results from a positive matrix factorization (PMF) analysis of these data, were used to understand the role of regional transport on SOC concentrations. A backward-trajectory analysis, coupled with the measurements and estimated source contributions, were used to evaluate the origins of SOC aerosols. Anthropogenic and biogenic SOC were identified in central LA over the study period, together contributing 40% of the annual average PM2.5 OC mass. There were distinct seasonal variations, with high contributions of anthropogenic SOC in summer, and high contributions of biogenic SOC in spring. The back-trajectory analysis, coupled with daily source contributions of SOC and organic compounds as indicators, allowed us to identify potential source locations and dominant meteorological conditions contributing to elevated SOC at the measurement site. The results show that air mass movements from the Pacific Ocean are associated with higher contributions of anthropogenic SOC to the PM2.5 OC in downtown LA, suggesting that the combination of local meteorological conditions and local anthropogenic emissions led to an increase in the anthropogenic SOC. In contrast, air masses passing over the Central Valley and forested areas where there are biogenic hydrocarbon emissions are closely associated with higher contributions of biogenic SOC in the region. The study emphasizes that higher anthropogenic SOC contributions are due to the combination of local emissions with humidity air from the ocean, and that higher biogenic SOC contributions are impacted by transport of pollutants from regions outside the LA Basin.

Meteorological controls on particle growth events in Beltsville, MD, USA during July 2011

During summer 2011, particle growth events were investigated in Beltsville, Maryland, USA where anthropogenic and biogenic hydrocarbon emissions heavily influenced the lower atmosphere. Aerosol sampling was made from a 5-m tower during July 2011. Ultrafine particle growth events occurred on 4 of the 25 days sampled. Regional particle growth events occurred after the passage of synoptic cold fronts. During regional particle growth events temperature and relative humidity were 2° Celsius lower and 3 % less than on non-event days and the local wind direction came from the northeast. With average growth rates of 3.5 nm hr−1, regional particle growth events happened around 15:00 Universal Time Coordinated, shortly after increased mixing within the atmospheric boundary layer. Regional particle growth events were associated with cooler, drier, mostly sunny days that had low sulfur dioxide mixing ratio (~0.6 parts per billion by volume). Regional particle growth events occurred when the atmospheric boundary layer was dominated by free convection and had lower sensible heat fluxes compared to short-lived events or non-particle growth event days.

Feedbacks between air pollution and weather, part 2: Effects on chemistry

Fully-coupled air-quality models running in “feedback” and “no-feedback” configurations were compared against each other and observation network data as part of Phase 2 of the Air Quality Model Evaluation International Initiative. In the “no-feedback” mode, interactions between meteorology and chemistry through the aerosol direct and indirect effects were disabled, with the models reverting to climatologies of aerosol properties, or a no-aerosol weather simulation, while in the “feedback” mode, the model-generated aerosols were allowed to modify the models' radiative transfer and/or cloud formation processes. Annual simulations with and without feedbacks were conducted for domains in North America for the years 2006 and 2010, and for Europe for the year 2010. Comparisons against observations via annual statistics show model-to-model variation in performance is greater than the within-model variation associated with feedbacks. However, during the summer and during intense emission events such as the Russian forest fires of 2010, feedbacks have a significant impact on the chemical predictions of the models.The aerosol indirect effect was usually found to dominate feedbacks compared to the direct effect. The impacts of direct and indirect effects were often shown to be in competition, for predictions of ozone, particulate matter and other species. Feedbacks were shown to result in local and regional shifts of ozone-forming chemical regime, between NOx- and VOC-limited environments. Feedbacks were shown to have a substantial influence on biogenic hydrocarbon emissions and concentrations: North American simulations incorporating both feedbacks resulted in summer average isoprene concentration decreases of up to 10%, while European direct effect simulations during the Russian forest fire period resulted in grid average isoprene changes of −5 to +12.5%. The atmospheric transport and chemistry of large emitting sources such as plumes from forest fires and large cities were shown to be strongly impacted by the presence or absence of feedback mechanisms in the model simulations. Summertime model performance for ozone and other gases was improved through the inclusion of indirect effect feedbacks, while performance for particulate matter was degraded, suggesting that current parameterizations for in- and below cloud processes, once the cloud locations become more directly influenced by aerosols, may over- or under-predict the strength of these processes. Process parameterization-level comparisons of fully coupled feedback models are therefore recommended for future work, as well as further studies using these models for the simulations of large scale urban/industrial and/or forest fire plumes.

Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX

Abstract. Organic compounds are a large component of aerosol mass, but organic aerosol (OA) sources remain poorly characterized. Recent model studies have suggested nighttime oxidation of biogenic hydrocarbons as a potentially large OA source, but analysis of field measurements to test these predictions is sparse. We present nighttime vertical profiles of nitrogen oxides, ozone, VOCs and aerosol composition measured during low approaches of the NOAA P-3 aircraft to airfields in Houston, TX. This region has large emissions of both biogenic hydrocarbons and nitrogen oxides. The latter category serves as a source of the nitrate radical, NO3, a key nighttime oxidant. Biogenic VOCs (BVOC) and urban pollutants were concentrated within the nocturnal boundary layer (NBL), which varied in depth from 100–400 m. Despite concentrated NOx at low altitude, ozone was never titrated to zero, resulting in rapid NO3 radical production rates of 0.2–2.7 ppbv h−1 within the NBL. Monoterpenes and isoprene were frequently present within the NBL and underwent rapid oxidation (up to 1 ppbv h−1), mainly by NO3 and to a lesser extent O3. Concurrent enhancement in organic and nitrate aerosol on several profiles was consistent with primary emissions and with secondary production from nighttime BVOC oxidation, with the latter equivalent to or slightly larger than the former. Some profiles may have been influenced by biomass burning sources as well, making quantitative attribution of organic aerosol sources difficult. Ratios of organic aerosol to CO within the NBL ranged from 14 to 38 μg m−3 OA/ppmv CO. A box model simulation incorporating monoterpene emissions, oxidant formation rates and monoterpene SOA yields suggested overnight OA production of 0.5 to 9 μg m−3.

MATHEMATICAL MODELS TO ESTIMATE THE MASS OF LEAF AND SKETCH THE SHAPE OF TREE

The mass of leaf is a key factor to estimate the magnitude of biogenic hydrocarbon emission. In this paper, following the minimum material consumption assumption and the conservation law of energy, we build a mathematical model to calculate the mass of leaf, crown and the whole tree, respectively. Also, we translate the shape of crown to match the solution of a second order differential equations with boundary value conditions. Meanwhile, we try to explore what does the climatic zone affect the shape and thickness of leaf. In the simulation section, by using the measured data for 14 trees in 3 different species, we present various simulation results through our models and formulas. Finally, following our models and formulas, we find out some hidden relationships: 1. There is an intrinsic link between the single leaf area and the hardness of the stem; 2. There is an interconnected relationship between the shape of leaf and the shape of tree; 3. There are lots of trees with large and thick leaves living in the torrid zone and few in the cold zone.

Nocturnal isoprene declines in a semi-urban environment

In environments dominated by biogenic hydrocarbon emissions, the transition from daytime to nighttime is an important period because ambient isoprene levels rapidly decrease. In sub-urban environments with abundant sources of nitrogen oxides, the nighttime isoprene chemistry has implications for the regional nitrogen oxide budget. Given the substantial production of alkyl nitrates from isoprene reactions during the nighttime, nitrogen oxides can then be transported long distances in the form of nitrates. The factors that influence nighttime chemistry of isoprene in environments with abundant sources of nitrogen oxides are not well known. Therefore, the objective of this study was to understand the processes controlling isoprene levels just before and after sunset, in an environment under the influences of moderate concentrations of ambient nitrogen oxides. Utilizing in-situ Proton-Transfer-Reaction Mass Spectrometer measurements, isoprene levels were studied during July to August 2011 in a sub-urban environment outside the metropolis of Washington, D.C., USA. Numerical modeling investigations were also pursued to determine yields of alkyl nitrates. Pre-sunset isoprene rises, observed on eight measured days, were likely related to the cessation of atmospheric turbulence and stabilization of the surface layer. After sunset, nocturnal declines of isoprene, while not fully explained by chemical reactions, depended on the amounts of nitrate radicals in the lower atmosphere. Furthermore, isoprene destruction rates and associated production of alkyl nitrates depended on the amounts of nitrogen oxides. Compared with cases with ambient nitrogen oxides lower than 10 parts per billion, model results showed that twice the amounts of isoprene were destroyed when average nitrogen oxide levels exceeded 30 parts per billion.

Spatial and seasonal variations of fine particle water-soluble organic carbon (WSOC) over the southeastern United States: implications for secondary organic aerosol formation

Abstract. Secondary organic aerosol (SOA) in the southeastern US is investigated by analyzing the spatial-temporal distribution of water-soluble organic carbon (WSOC) and other PM2.5 components from 900 archived 24-h Teflon filters collected at 15 urban or rural EPA Federal Reference Method (FRM) network sites throughout 2007. Online measurements of WSOC at an urban/rural-paired site in Georgia in the summer of 2008 are contrasted to the filter data. Based on FRM filters, excluding biomass-burning events (levoglucosan < 50 ng m−3), WSOC and sulfate were highly correlated with PM2.5 mass (r2~0.7). Both components comprised a large mass fraction of PM2.5 (13% and 31%, respectively, or ~25% and 50% for WSOM and ammonium sulfate). Sulfate and WSOC both tracked ambient temperature throughout the year, suggesting the temperature effects were mainly linked to faster photochemistry and/or synoptic meteorology and less due to enhanced biogenic hydrocarbon emissions. FRM WSOC, and to a lesser extent sulfate, were spatially homogeneous throughout the region, yet WSOC was moderately enhanced (27%) in locations of greater predicted isoprene emissions in summer. A Positive Matrix Factorization (PMF) analysis identified two major source types for the summer WSOC; 22% of the WSOC were associated with ammonium sulfate, and 56% of the WSOC were associated with brown carbon and oxalate. A small urban excess of FRM WSOC (10%) was observed in the summer of 2007, however, comparisons of online WSOC measurements at one urban/rural pair (Atlanta/Yorkville) in August 2008 showed substantially greater difference in WSOC (31%) relative to the FRM data, suggesting a low bias for urban filters. The measured Atlanta urban excess, combined with the estimated boundary layer heights, gave an estimated Atlanta daily WSOC production rate in August of 0.55 mgC m−2 h−1 between mid-morning and mid-afternoon. This study characterizes the regional nature of fine particles in the southeastern US, confirming the importance of SOA and the roles of both biogenic and anthropogenic emissions.

The contribution of organics to atmospheric nanoparticle growth

The growth of the smallest atmospheric particles to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. A synthesis of research indicates that the mechanisms controlling this growth depend on the size of the growing particle. Aerosols have a strong, yet poorly quantified, effect on climate. The growth of the smallest atmospheric particles from diameters in the nanometre range to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. In many environments, atmospheric nanoparticles grow by taking up organic compounds that are derived from biogenic hydrocarbon emissions. Several mechanisms may control this uptake. Condensation of low-volatility vapours and formation of organic salts probably dominate the very first steps of growth in particles close to 1 nm in diameter. As the particles grow further, formation of organic polymers and effects related to the phase of the particle probably become increasingly important. We suggest that dependence of particle growth mechanisms on particle size needs to be investigated more systematically.

Hydroxyl radicals in the tropical troposphere over the Suriname rainforest: airborne measurements

Abstract. Direct measurements of OH and HO2 over a tropical rainforest were made for the first time during the GABRIEL campaign in October 2005, deploying the custom-built HORUS instrument (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy), adapted to fly in a Learjet wingpod. Biogenic hydrocarbon emissions were expected to strongly reduce the OH and HO2 mixing ratios as the air is transported from the ocean over the forest. However, surprisingly high mixing ratios of both OH and HO2 were encountered in the boundary layer over the rainforest. The HORUS instrumentation and calibration methods are described in detail and the measurement results obtained are discussed. The extensive dataset collected during GABRIEL, including measurements of many other trace gases and photolysis frequencies, has been used to quantify the main sources and sinks of OH. Comparison of these measurement-derived formation and loss rates of OH indicates strong previously overlooked recycling of OH in the boundary layer over the tropical rainforest, occurring in chorus with isoprene emission.

Attribution of projected changes in summertime US ozone and PM<sub>2.5</sub> concentrations to global changes

Abstract. The impact that changes in future climate, anthropogenic US emissions, background tropospheric composition, and land-use have on summertime regional US ozone and PM2.5 concentrations is examined through a matrix of downscaled regional air quality simulations, where each set of simulations was conducted for five months of July climatology, using the Community Multi-scale Air Quality (CMAQ) model. Projected regional scale changes in meteorology due to climate change under the Intergovernmental Panel on Climate Change (IPCC) A2 scenario are derived through the downscaling of Parallel Climate Model (PCM) output with the MM5 meteorological model. Future chemical boundary conditions are obtained through downscaling of MOZART-2 (Model for Ozone and Related Chemical Tracers, version 2.4) global chemical model simulations based on the IPCC Special Report on Emissions Scenarios (SRES) A2 emissions scenario. Projected changes in US anthropogenic emissions are estimated using the EPA Economic Growth Analysis System (EGAS), and changes in land-use are projected using data from the Community Land Model (CLM) and the Spatially Explicit Regional Growth Model (SERGOM). For July conditions, changes in chemical boundary conditions are found to have the largest impact (+5 ppbv) on average daily maximum 8-h (DM8H) ozone. Changes in US anthropogenic emissions are projected to increase average DM8H ozone by +3 ppbv. Land-use changes are projected to have a significant influence on regional air quality due to the impact these changes have on biogenic hydrocarbon emissions. When climate changes and land-use changes are considered simultaneously, the average DM8H ozone decreases due to a reduction in biogenic VOC emissions (−2.6 ppbv). Changes in average 24-h (A24-h) PM2.5 concentrations are dominated by projected changes in anthropogenic emissions (+3 μg m−3), while changes in chemical boundary conditions have a negligible effect. On average, climate change reduces A24-h PM2.5 concentrations by −0.9 μg m−3, but this reduction is more than tripled in the Southeastern US due to increased precipitation and wet deposition.

Correcting photolysis rates on the basis of satellite observed clouds

Clouds can significantly affect photochemical activities in the boundary layer by altering radiation intensity, and therefore their correct specification in the air quality models is of outmost importance. In this study we introduce a technique for using the satellite observed clouds to correct photolysis rates in photochemical models. This technique was implemented in EPA's Community Multiscale Air Quality modeling system (CMAQ) and was tested over a 10 day period in August 2000 that coincided with the Texas Air Quality Study (TexAQS). The simulations were performed at 4 and 12 km grid size domains over Texas, extending east to Mississippi, for the period of 24 to 31 August 2000. The results clearly indicate that inaccurate cloud prediction in the model can significantly alter the predicted atmospheric chemical composition within the boundary layer and exaggerate or underpredict ozone concentration. Cloud impact is acute and more pronounced over the emission source regions and can lead to large errors in the model predictions of ozone and its by‐products. At some locations the errors in ozone concentration reached as high as 60 ppb which was mostly corrected by the use of our technique. Clouds also increased the lifetime of ozone precursors leading to their transport out of the source regions and causing further ozone production down‐wind. Longer lifetime for nitrogen oxides (NOx = NO + NO2) and its transport over regions high in biogenic hydrocarbon emissions (in the eastern part of the domain) led to increased ozone production that was missing in the control simulation. Over Houston‐Galveston Bay area, the presence of clouds altered the chemical composition of the atmosphere and reduced the net surface removal of reactive nitrogen compounds. Use of satellite observed clouds significantly improved model predictions in areas impacted by clouds. Errors arising from an inconsistency in the cloud fields can impact the performance of photochemical models used for case studies as well as for air quality forecasting. Air quality forecast models often use the model results from the previous forecast (or some adjusted form of it) for the initialization of the new forecast. Therefore such errors can propagate into the future forecasts, and the use of observed clouds in the preparation of initial concentrations for air quality forecasting could be beneficial.

Regional climate change and its impact on photooxidant concentrations in southern Germany: Simulations with a coupled regional climate‐chemistry model

In order to investigate possible effects of global climate change on the near‐surface concentrations of photochemical compounds in southern Germany, nested regional simulations with a coupled climate‐chemistry model were carried out. The simulations with a horizontal resolution of 60 km for Europe and 20 km for central Europe were driven by meteorological boundary conditions provided by a long‐term simulation of the global climate model ECHAM4. Two time slices of about 10 years were compared, one representing the 1990s and one representing the 2030s. For the region of southern Germany the simulations show an increase of the mean summer temperature by almost 2° along with a decrease of cloud water and ice and a corresponding increase of the photolysis frequencies and the emissions of biogenic hydrocarbons. Under the model assumption of unchanged anthropogenic emissions this leads to an increase of the mean mixing ratios of most photooxidants. Because of the complex topography and the heterogeneous distribution of precursor emissions all parameters show pronounced regional patterns. The average daily maximum ozone concentrations in southern Germany increase for the considered scenario by nearly 10% in the summer months. Depending on the region, the increase of the mean daily maximum ranges between 2 and 6 ppb. As a consequence, the number of days when the 8‐hour mean of the ozone concentration exceeds the threshold value of 120 μg m−3 increases by 5 to 12 days per year.

Role of climate change in global predictions of future tropospheric ozone and aerosols

A unified tropospheric chemistry‐aerosol model within the Goddard Institute for Space Studies general circulation model II′ is applied to simulate an equilibrium CO2‐forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5–20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2‐driven climate change alone is predicted to reduce the global O3 burden as a result of faster removal of O3 in a warmer climate, it is predicted to increase surface layer O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate‐sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate‐induced changes in burdens and different climatological conditions; with full gas‐aerosol coupling and accounting for ozone and aerosols from both natural and anthropogenic sources, year 2100 global mean top of the atmosphere direct radiative forcings by O3, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, −0.72, −1.0, +1.26, and −0.56 W m−2, respectively, using present‐day climate and year 2100 emissions, while they are predicted to be +0.76, −0.72, −0.74, +0.97, and −0.58 W m−2, respectively, with year 2100 climate and emissions.

NO emissions from large point sources: variability in ozone production, resulting health damages and economic costs

We present a proof-of-concept analysis of the measurement of the health damage of ozone (O3) produced from nitrogen oxides (NOx=NO+NO2) emitted by individual large point sources in the eastern United States. We use a regional atmospheric model of the eastern United States, the Comprehensive Air quality Model with Extensions (CAMx), to quantify the variable impact that a fixed quantity of NOx emitted from individual sources can have on the downwind concentration of surface O3, depending on temperature and local biogenic hydrocarbon emissions. We also examine the dependence of resulting O3-related health damages on the size of the exposed population. The investigation is relevant to the increasingly widely used “cap and trade” approach to NOx regulation, which presumes that shifts of emissions over time and space, holding the total fixed over the course of the summer O3 season, will have minimal effect on the environmental outcome. By contrast, we show that a shift of a unit of NOx emissions from one place or time to another could result in large changes in resulting health effects due to O3 formation and exposure. We indicate how the type of modeling carried out here might be used to attach externality-correcting prices to emissions. Charging emitters fees that are commensurate with the damage caused by their NOx emissions would create an incentive for emitters to reduce emissions at times and in locations where they cause the largest damage.

Charging Nox Emitters for Health Damages: An Exploratory Analysis

We present a proof-of-concept analysis of the measurement of the health damage of ozone (O3) produced from nitrogen oxides (NOx = NO + NO2) emitted by individual large point sources in the eastern United States. We use a regional atmospheric model of the eastern United States, the Comprehensive Air Quality Model with Extensions (CAMx), to quantify the variable impact that a fixed quantity of NOx emitted from individual sources can have on the downwind concentration of surface O3, depending on temperature and local biogenic hydrocarbon emissions. We also examine the dependence of resulting ozone-related health damages on the size of the exposed population. The investigation is relevant to the increasingly widely used ?cap and trade? approach to NOx regulation, which presumes that shifts of emissions over time and space, holding the total fixed over the course of the summer O3 season, will have minimal effect on the environmental outcome. By contrast, we show that a shift of a unit of NOx emissions from one place or time to another could result in large changes in the health effects due to ozone formation and exposure. We indicate how the type of modeling carried out here might be used to attach externality-correcting prices to emissions. Charging emitters fees that are commensurate with the damage caused by their NOx emissions would create an incentive for emitters to reduce emissions at times and in locations where they cause the largest damage.