Variations of the increasing trend of tropospheric NO2 over central east China during the past decade

A numerical analysis using a regional chemical transport model (CTM) is presented in comparison with Global Ozone Monitoring Experiment (GOME) and SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) satellite NO₂ measurements over East Asia from 1996 to 2005 from a climatological perspective. Modeling results agree well with satellite retrievals in geographical distribution patterns, with systematic underestimation of the absolute values. The sharp increase in NO₂ vertical column densities (VCDs) over central east China (CEC) after the year 2000 (14.1–20.5% yr⁻¹ for the satellite observations and 10.8% yr⁻¹ for model simulations) is analyzed quantitatively over different megacity clusters. The distinct emission increase patterns are responsible for the different increase trends observed over the Beijing megacity cluster (BJ), the Yangtze Delta (YD) and other CEC regions. The growth rate of satellite measured and CMAQ-modeled NO₂ VCDs for the YD is much higher than that in other regions, with no clear seasonal variation. Apart from BJ and YD, NO₂ emissions from other regions in CEC also expand considerably.     

Comparison of satellite observed tropospheric NO2 over India with model simulations

Nitrogen dioxide (NO₂) plays a key role in the chemistry of the atmosphere and is emitted mainly by combustion processes. These emissions have been increasing over India over the past few years due to rapid economic growth and yet there are very few systematic ground based observations of NO₂ over this region. We thus take recourse to satellite data and compare tropospheric NO₂ column abundances simulated by a chemical transport model, MOZART, with data from the Global Ozone Monitoring Experiment (GOME) for a few locations in India that have seen a rapid economic growth in the last decade. The model generally simulates higher columnar abundances of NO₂ compared to GOME observations and does not reproduce the features of the observed seasonal behaviour. The combined uncertainties of the emission inventory and retrieval of the satellite data could be contributing factors to the discrepancies. It may be thus worthwhile to develop emission inventories for India at a higher resolution to include local level activity data. The ten year data (1996–2006) from GOME and SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) show increasing trends for Indian cities where rapid industrial and vehicular traffic growth has been observed during this period.     

Cost of lower NOx emissions: Increased CO2 emissions from heavy-duty diesel engines

This paper highlights the effect of emissions regulations on in-use emissions from heavy-duty vehicles powered by different model year engines. More importantly, fuel economy data for pre- and post-consent decree engines are compared.The objective of this study was to determine the changes in brake-specific emissions of NO_x as a result of emission regulations, and to highlight the effect these have had on brake-specific CO₂ emission; hence, fuel consumption. For this study, in-use, on-road emission measurements were collected. Test vehicles were instrumented with a portable on-board tailpipe emissions measurement system, WVU's Mobile Emissions Measurement System, and were tested on specific routes, which included a mix of highway and city driving patterns, in order to collect engine operating conditions, vehicle speed, and in-use emission rates of CO₂ and NO_x. Comparison of on-road in-use emissions data suggests NO_x reductions as high as 80% and 45% compared to the US Federal Test Procedure and Not-to-Exceed standards for model year 1995–2002. However, the results indicate that the fuel consumption; hence, CO₂ emissions increased by approximately 10% over the same period, when the engines were operating in the Not-to-Exceed region.     

Trend analysis of urban NO2 concentrations and the importance of direct NO2 emissions versus ozone/NOx equilibrium

The annual air quality standard of NO₂ is often exceeded in urban areas near heavy traffic locations. Despite significant decrease of NO_x emissions in 1986–2005 in the industrial and harbour area near Rotterdam, NO₂ concentrations at the urban background remain at the same level since the end of the nineties. Trend analysis of monitoring data revealed that the ozone/NO_x equilibrium is a more important factor than increasing direct NO₂ emissions by traffic. The latter has recently been identified as an additional NO₂ source due to the introduction of oxy-catalytic converters in diesel vehicles and the growing number of diesel vehicles. However, in Rotterdam over the period 1986–2005 direct NO₂ emissions by road traffic only increased 3–4%. Due to the importance of the ozone/NO_x equilibrium, it is concluded that local NO_x emissions in Rotterdam need substantial reduction to achieve lower NO₂ urban background levels. This is a relatively costly abatement strategy and, therefore, a “hotspot” approach aiming at reducing NO_x emissions by local traffic measures is more effective to meet European air quality standards.     

Pollution events over the East Mediterranean: Synergistic use of GOME,ground-based and sonde observations and models

The behaviour of ozone (O₃) and two important precursors, nitrogen dioxide (NO₂) and formaldehyde (HCHO), over the East Mediterranean in spring from 1996 to 2002 is studied in order to characterise the buildup of tropospheric O₃. The vertical distribution of O₃ observed over Crete during the Photochemical Activity and Solar Ultraviolet Radiation (PAUR II) campaign in May 1999 has been used for validation of satellite-derived data. Retrievals of O₃ columns from measurements of backscattered radiation by Global Ozone Monitoring Experiment (GOME) are compared with Total Ozone Mapping Spectrometer (TOMS), balloon, Systeme d’Analyse par Observation Zenithale (SAOZ) and LIDAR observations. The total O₃ vertical columns vary between 270 and 402 DU and correlate well with changes in air circulation patterns. The total observed variability in tropospheric O₃ is about 25 DU. Chemical box model calculations associate the GOME-observed NO₂ and HCHO tropospheric columns with a potential of daily photochemical enhancement in the tropospheric O₃ columns of about 0.8–1 DU over Crete and estimate the daily potential of regional photochemical buildup within upwind polluted air masses at about 2–8 DU. A Langrangian analysis attributes at most 10–20 DU of tropospheric O₃ to stratosphere–troposphere exchange (STE). The remainder is attributed to long-range transport of O₃ from industrial regions in Central Europe. From 1996 to 2002, in May no significant inter-annual variation in the tropospheric NO₂ and HCHO columns over Crete has been observed by GOME suggesting no detectable increase in regionally produced tropospheric O₃.     

Influence of model grid resolution on NO2 vertical column densities over East Asia

NO₂ vertical column densities (VCDs) over East Asia in June and December 2007 were simulated by the Community Multi-scale Air Quality (CMAQ) version 4.7.1 using an updated and more elaborate version of the Regional Emission Inventory in Asia (REAS) version 2. The modeling system could reasonably capture observed spatiotemporal changes of NO₂ VCDs by satellite sensors, the Global Ozone Monitoring Experiment-2 (GOME-2), the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY), and the Ozone Monitoring Instrument (OMI), even at the coarsest horizontal resolution of 80 km. The CMAQ simulations were performed in a sequence of three horizontal resolutions (80 km, 40 km, and 20 km) for June and December 2007 to investigate the influence of changes of horizontal resolution on the obtained NO₂ VCDs. CMAQ-simulated NO₂ VCDs generally increased with improvements in resolution from 80 km to 40 km and then to 20 km. Increases in the CMAQ-simulated NO₂ VCDs were greater for the change from 80 km to 40 km than for those from 40 km and 20 km, in which the increases of NO₂ VCDs due to the improvement of horizontal resolution were approached convergence at the horizontal resolution of approximately 20 km. Conversely, no clear convergences in NO₂ VCDs changes were found at near Tokyo and over the East China Sea. The biases of the NO₂ VCDs simulated at a resolution of 20 km against the satellite retrievals were ～36% near Beijing (CHN1) and ～78% near Shanghai (CHN2) in summer; these errors were found to be comparable to the horizontal resolution-dependent errors, which were 18–25% at CHN1 and 44–58% at CHN2 from 80 km to 40 km. Conversely, the influence of changes of horizontal resolution in winter was relatively less compared to that in summer.

Implications: NO₂ VCDs over East Asia in June and December 2007 were simulated using CMAQ version 4.7.1 and REAS version 2. The modeling system could reasonably capture observed spatiotemporal changes of NO₂ VCDs by satellite sensors. The CMAQ simulations were performed in a sequence of three horizontal resolutions, 80, 40, and 20 km, to investigate the influence of changes of horizontal resolution on the obtained NO₂ VCDs. The results suggested that the influence of changes of horizontal resolution was larger in summer compared to that in winter. The magnitude of the influence was comparable to the biases of the NO₂ VCDs simulated at a resolution of 20 km against the satellite retrievals.     

Modeling Analyses of the Effects of Changes in Nitrogen Oxides Emissions from the Electric Power Sector on Ozone Levels in the Eastern United States

Abstract

In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NO_x) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NO_x emissions reductions imposed on the utility sector by the NO_x State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NO_x emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NO_x SIP Call. Comparison of the “no-control” with the “2002” scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NO_x emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.     

Traffic pollution in a downtown site of Buenos Aires City

It has recently been recognized that air and noise pollution constitutes an extended problem over the densely populated city of Buenos Aires. Traffic emissions are of paramount concern, especially along narrow and main traffic arteries. In spite of these considerations, few systematic studies have been undertaken to evaluate the air quality in the metropolitan area of the city. In 1996, concentrations of carbon monoxide (CO), nitric oxide (NO), nitrogen dioxide (NO₂) and ozone (O₃) were simultaneously measured for the first time using a continuous monitoring station. This station was placed in a building at Belgrano Avenue, which is a heavy traffic street in the downtown area of the city (Bogo et al., Atmospheric Environment 33 (1999) 2587. In this work, we analyze the dependence of the measured primary pollutants, CO and the mixture of nitrogen oxides (NO_x), with meteorological conditions, traffic emissions and monitoring location. We compare the registered values with the results obtained from modeling the dispersion of the pollutants emitted from mobile and area sources. We also discuss the relevance of street canyon effects compared with background concentrations of these pollutants.     

Climatic forcing of nitrogen oxides through changes in tropospheric ozone and methane; global 3D model studies

A three-dimensional global chemical tracer model and a radiation transfer model have been used to study the role of NO_x emissions for radiative forcing of climate. Through production of tropospheric O₃, NO_x emissions lead to positive radiative forcing and warming. But by affecting the concentration of OH radicals, NO_x also reduces the levels of CH₄, thereby giving negative forcing and cooling. The lifetime of NO_x varies from hours to days, giving large spatial variations in the levels of NO_x. We have selected geographical regions representing different chemical and physical conditions, and chemical and radiative effects of reducing NO_x emissions by 20% in each region are studied. Due to nonlinearities in the O₃ chemistry as well as differences in convective activity, there are large geographical differences in the effect of NO_x on O₃ as well as variations in the annual profile of the changes. The effect of NO_x emissions on methane is also found to depend on the localisation of the emissions. The calculated ozone and methane forcing are of similar magnitude but of opposite sign. The methane effect acts on a global scale with a delay of approximately a decade, while the ozone effect is of regional character and occurs during weeks.     

Automated Chemical Mass Balance Receptor Modeling

Abstract

A nontrivial portion of heavy-duty vehicle emissions of NO_x and particulate matter (PM) occurs during idling. Regulators and the environmental community are interested in curtailing truck idling emissions, but current emissions models do not characterize them accurately, and little quantitative data exist to evaluate the relative effectiveness of various policies. The objectives of this study were to quantify the effect of accessory loading and engine speed on idling emissions from a properly functioning, modern, heavy-duty diesel truck and to compare these results with data from earlier model year vehicles. It was found that emissions during idling varied greatly as a function of engine model year, engine speed, and accessory load conditions. For the 1999 model year Class 8 truck tested, raising the engine speed from 600 to 1050 rpm and turning on the air conditioning resulted in a 2.5-fold increase in NO_x emissions in grams per hour, a 2-fold increase in CO₂ emissions, and a 5-fold increase in CO emissions while idling. On a grams per gallon fuel basis, NO_x emissions while idling were approximately twice as high as those at 55 mph. The CO₂ emissions at the two conditions were closer. The NO_x emissions from the 1999 truck while idling with air conditioning running were slightly more than those of two 1990 model year trucks under equivalent conditions, and the hydrocarbon (HC) and CO emissions were significantly lower. It was found that the NO_x emissions used in the California Air Resources Board’s (CARB) EMFAC2000 and the U.S. Environmental Protection Agency’s (EPA) MOBILE5b emissions inventory models were lower than those measured in all of the idling conditions tested on the 1999 truck.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Characterizations of chemical oxidants in Mexico City: A regional chemical dynamical model (WRF-Chem) study

The formation of chemical oxidants, particularly ozone, in Mexico City were studied using a newly developed regional chemical/dynamical model (WRF-Chem). The magnitude and timing of simulated diurnal cycles of ozone (O₃), carbon monoxide (CO) and nitrogen oxides (NO_x)_, and the maximum and minimum O₃ concentrations are generally consistent with surface measurements. Our analysis shows that the strong diurnal cycle in O₃ is mainly attributable to photochemical variations, while diurnal cycles of CO and NO_x mainly result from variations of emissions and boundary layer height. In a sensitivity study, oxidation reactions of aromatic hydrocarbons (HCs) and alkenes yield highest peak O₃ production rates (20 and 18 ppbv h⁻¹, respectively). Alkene oxidations, which are generally faster, dominate in early morning. By late morning, alkene concentrations drop, and oxidations of aromatics dominate, with lesser contributions from alkanes and CO. The sensitivity of O₃ concentrations to NO_x and HC emissions was assessed. Our results show that daytime O₃ production is HC-limited in the Mexico City metropolitan area, so that increases in HC emissions increase O₃ chemical production, while increases in NO_x emissions decrease O₃ concentrations. However, increases in both NO_x and HC emissions yield even greater O₃ increases than increases in HCs alone. Uncertainties in HC emissions estimates give large uncertainties in calculated daytime O₃, while NO_x emissions uncertainties are less influential. However, NO_x emissions are important in controlling O₃ at night.     

Modelling NOx from lightning and its impact on global chemical fields

We have used a three-dimensional off-line chemical transport model (CTM) to assess the impact of lightning emissions in the free troposphere both on NO_x itself and on other chemical species such as O₃ and OH. We have investigated these effects using two lightning emission scenarios. In the first, lightning emissions are coupled in space and time to the convective cloud top height calculated every 6 h by the CTM's moist convection scheme. In the second, lightning emissions are calculated as a constant, monthly mean field. The model's performance against observed profiles of NO_x and O₃ in the Atlantic and Pacific ocean improves significantly when lightning emissions are included. With the inclusion of these emissions, the CTM produces a significant increase in the NO_x concentrations in the upper troposphere, where the NO_x lifetime is long, and a smaller increase in the lower free troposphere, where the surface NO_x sources dominate. These changes cause a significant increase in the O₃ production in the upper troposphere and hence higher calculated O₃ there. The model indicates that lightning emissions cause local increases of over 50 parts per 10¹² by volume (pptv) in NO_x, 200 pptv in HNO₃ and 20 parts per 10⁹ by volume (ppbv) (>40%) in O₃. In addition, a smaller increase of O₃ in the lower troposphere occurs due to an increase in the downward transport of O₃. The O₃ change is accompanied by an increase in OH which is more pronounced in the upper troposphere with a corresponding reduction in CO. The method of emission employed in the model does not appear to have a significant effect globally. In the upper troposphere (above about 300 hPa) NO_x concentrations are generally lower with monthly mean emissions, because of the de-coupling of emissions from the model's convection scheme, which vents NO_x aloft more efficiently in the coupled scheme. Below the local convective outflow altitude, NO_x concentrations are larger when using the monthly mean emissions than when coupled to the convection scheme, because the more dilute emissions, and nighttime emissions, lead to a slower NO_x destruction rate. Only minor changes are predicted in the monthly average fields of O₃ if we emit lightning as a monthly constant field. However, the method of emission becomes important when we make a direct comparison of model results with time varying data. These differences should be taken into account when a direct comparison of O₃ with measurements collected at particular times and locations is attempted.     

Air pollution at a hotspot location in Delhi: Detecting trends,seasonal cycles and oscillations

This paper uses spectral methods to analyze changes in air quality at a single monitoring site in Delhi since 2000. Power spectral density calculations of daily concentration data for particulate matter (PM10), carbon monoxide (CO), oxides of nitrogen (NO_x) and oxides of sulfur (SO_x) reveal the presence of trends and periodic oscillations for all the pollutants. Singular Spectrum Analysis (SSA) is used to decompose daily data into statistically significant non-linear trends, seasonal cycles and other oscillations. Periods of sharp reductions were observed for both SO_x and CO concentrations in 2001 and 2002, respectively. NO_x concentration trends show a sustained rise from 2000 to 2004, followed by small decline thereafter. PM10 concentration trends remain essentially unchanged over the time period. All pollutants also show strong annual and biannual cycles. The observed trends in CO and NO_x likely relate changes in Delhi's vehicular traffic emissions. The sharp drop in both the trend and amplitude of the seasonal cycle of CO coincides with the switch to Compressed Natural Gas (CNG) as a fuel for Delhi's public transport fleet. Observed changes in SO_x and PM10 concentrations were most likely caused by sources unrelated to vehicular traffic.     

Idle Emissions from Heavy-Duty Diesel and Natural Gas Vehicles at High Altitude

ABSTRACT

Idle emissions of total hydrocarbon (THC), CO, NO_x, and particulate matter (PM) were measured from 24 heavy-duty diesel-fueled (12 trucks and 12 buses) and 4 heavy-duty compressed natural gas (CNG)-fueled vehicles. The volatile organic fraction (VOF) of PM and aldehyde emissions were also measured for many of the diesel vehicles. Experiments were conducted at 1609 m above sea level using a full exhaust flow dilution tunnel method identical to that used for heavy-duty engine Federal Test Procedure (FTP) testing. Diesel trucks averaged 0.170 g/min THC, 1.183 g/min CO, 1.416 g/min NO_x, and 0.030 g/min PM. Diesel buses averaged 0.137 g/min THC, 1.326 g/min CO, 2.015 g/min NO_x, and 0.048 g/min PM.

Results are compared to idle emission factors from the MOBILE5 and PART5 inventory models. The models significantly (45-75%) overestimate emissions of THC and CO in comparison with results measured from the fleet of vehicles examined in this study. Measured NO_x emissions were significantly higher (30-100%) than model predictions. For the pre-1999 (pre-consent decree) truck engines examined in this study, idle NO_x emissions increased with Health and Environment; June 30, 1999 (available from the authors).     

Anthropogenic NOx emissions in Asia in the period 1990–2020

Nitrogen oxides emissions in Asia during the period 1990–2020 due to anthropogenic activity are presented. These estimates are based on the RAINS-ASIA methodology (Foell et al., 1995, Acid Rain and Emission Reduction in Asia, World Bank), which includes a dynamic model for energy forecasts, and information on 6 energy sectors and 9 fuel types. The energy forecasts are combined with process emission factors to yield NO_x emission estimates at the country level, the regional level, and on a 1 degree by 1 degree grid. In 1990 the total NO_x emissions are estimated to be ∼19 Tg NO₂, with China (43%), India (18%) and Japan (13%) accounting for 75% of the total. Emissions by fuel are dominated by burning of hard coal and emissions by economic activity are dominated by the power, transport, and industrial sectors. These new estimates of NO_x emissions are compared with those published by Hameed and Dignon (1988, Atmospheric Environment 22, 441–449) and Akimoto and Narita (1994, Atmospheric Environment 28, 213–225). Future emissions under a no-further-control scenario are also presented. During the period 1990–2020 the NO_x emissions increase by 350%, to ∼86 Tg NO₂. The increase in NO_x emissions by sector and end-use varies between countries, but in all countries this increase is strongest in the power and transport sectors. These results highlight the dynamic nature of energy use in Asia, and the need to take the rapid growth in NO_x emissions in Asia into account in studies of air pollution and atmospheric chemistry.     

Sensitivity of ozone concentrations to diurnal variations of surface emissions in Mexico City: A WRF/Chem modeling study

Sensitivity of ozone (O₃) concentrations in the Mexico City area to diurnal variations of surface air pollutant emissions is investigated using the WRF/Chem model. Our analysis shows that diurnal variations of nitrogen oxides (NO_x = NO + NO₂) and volatile organic compound (VOC) emissions play an important role in controlling the O₃ concentrations in the Mexico City area. The contributions of NO_x and VOC emissions to daytime O₃ concentrations are very sensitive to the morning emissions of NO_x and VOCs. Increase in morning NO_x emissions leads to decrease in daytime O₃ concentrations as well as the afternoon O₃ maximum, while increase in morning VOC emissions tends to increase in O₃ concentrations in late morning and early afternoon, indicating that O₃ production in Mexico City is under VOC-limited regime. It is also found that the nighttime O₃ is independent of VOCs, but is sensitive to NO_x. The emissions of VOCs during other periods (early morning, evening, and night) have only small impacts on O₃ concentrations, while the emissions of NO_x have important impacts on O₃ concentrations in the evening and the early morning.This study suggests that shifting emission pattern, while keeping the total emissions unchanged, has important impacts on air quality. For example, delaying the morning emission peak from 8 am to 10 am significantly reduced the morning peaks of NO_x and VOCs, as well as the afternoon O₃ maxima. It suggests that without reduction of total emission, the daytime O₃ concentrations can be significantly reduced by changing the diurnal variations of the emissions of O₃ precursors.     

Source apportionment of fine particles utilizing partially speciated carbonaceous aerosol data at two rural locations in New York State

A source apportionment study was conducted at two rural locations, Potsdam and Stockton, to assess the in-state/out-of-state sources of PM_2.5 and Hg in New York State. At both locations, samples were collected between November 2002 and August 2005 and analyzed for fine PM mass and its chemical constituents. The measured chemical constituents included elements, cations, anions, organic and elemental carbon (OC and EC), black carbon (BC), and water-soluble short-chain (WSSC) organic acids. Positive matrix factorization (PMF) was applied to the measured concentrations and eight and seven factors were resolved at Potsdam and Stockton, respectively. Four factors were resolved in common between the two locations including secondary sulfate, secondary nitrate, secondary OC, and a crustal factor. The factor profiles of mixed industrial and motor vehicle factors resolved at Potsdam were different compared with the corresponding profiles for these factors at Stockton. A resuspended road salt factor was identified at Potsdam, while an aged sea salt factor was identified at Stockton. At Potsdam, a wood smoke factor was also resolved. Among the resolved factors, secondary sulfate was the highest contributor to the measured mass at both sites. Potential source contribution function (PSCF) analysis indicated the Ohio River Valley region as a common potential source region for this factor at both locations. For the secondary nitrate factor, at Potsdam PSCF analysis indicated the Midwestern US (NO_x emissions), and the US farm belt (ammonia emissions) as potential source regions, while at Stockton, the Midwestern US (power plant NO_x emissions) was indicated as a major potential source region.     

A Comprehensive Inventory of the Ship Traffic Exhaust Emissions in the Baltic Sea from 2006 to 2009

This study addresses the exhaust emissions of CO₂, NO_x, SO_x, CO, and PM_2.5 originated from Baltic Sea shipping in 2006–2009. Numerical results have been computed using the Ship Traffic Emissions Assessment Model. This model is based on the messages of the automatic identification system (AIS), which enable the positioning of ships with a high spatial resolution. The NO_x emissions in 2009 were approximately 7 % higher than in 2006, despite the economic recession. However, the SO_x emissions in 2009 were approximately 14 % lower, when compared to those in 2006, mainly caused by the fuel requirements of the SO_x emission control area (SECA) which became effective in May 2006, but affected also by changes in ship activity. Results are presented on the differential geographic distribution of shipping emissions before (Jan–April 2006) and after (Jan–April 2009) the SECA regulations. The predicted NO_x emissions in 2009 substantially exceeded the emissions in 2006 along major ship routes and at numerous harbors, mostly due to the continuous increase in the number of small vessels that use AIS transmitters. Although the SO_x emissions have been reduced in 2009 in most major ship routes, these have increased in the vicinity of some harbors and on some densely trafficked routes. A seasonal variation of emissions is also presented, as well as the distribution of emissions in terms of vessel flag state, type, and weight.     

Effects of uncertainty in the reaction of the hydroxyl radical with nitrogen dioxide on model-simulated ozone control strategies

We evaluated the effect of a 20% reduction in the rate constant of the reaction of the hydroxyl radical with nitrogen dioxide to produce nitric acid (OH+NO₂→HNO₃) on model predictions of ozone mixing ratios ([O₃]) and the effectiveness of reductions in emissions of volatile organic compounds (VOC) and nitrogen oxides (NO_x) for reducing [O₃]. By comparing a model simulation with the new rate constant to a base case scenario, we found that the [O₃] increase was between 2 and 6% for typical rural conditions and between 6 and 16% for typical urban conditions. The increases in [O₃] were less than proportional to the reduction in the OH+NO₂ rate constant because of negative feedbacks in the photochemical mechanism. Next, we used two different approaches to evaluate how the new OH+NO₂ rate constant changed the effectiveness of reductions in emissions of VOC and NO_x: first, we evaluated the effect on [O₃] sensitivity to small changes in emissions of VOC (d[O₃]/dE_VOC) and NO_x (d[O₃]/dE_NOx); and secondly, we used the empirical kinetic modeling approach to evaluate the effect on the level of emissions reduction necessary to reduce [O₃] to a specified level. Both methods showed that reducing the OH+NO₂ rate constant caused control strategies for VOC to become less effective relative to NO_x control strategies. We found, however, that d[O₃]/dE_VOC and d[O₃]/dE_NOx did not quantitatively predict the magnitude of the change in the control strategy because the [O₃] response was nonlinear with respect to the size of the emissions reduction. We conclude that model sensitivity analyses calculated using small emissions changes do not accurately characterize the effect of uncertainty in model inputs (in this case, the OH+NO₂ rate constant) on O₃ attainment strategies. Instead, the effects of changes in model inputs should be studied using large changes in precursor emissions to approximate realistic attainment scenarios.