Development of a speciated, hourly, and gridded air pollutants emission modeling system--a case study on the precursors of photochemical smog in the Seoul metropolitan area, Korea

A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas. The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.     

Rural southeast Texas air quality measurements during the 2006 Texas Air Quality Study

The authors conducted air quality measurements of the criteria pollutants carbon monoxide, nitrogen oxides, and ozone together with meteorological measurements at a park site southeast of College Station, TX, during the 2006 Texas Air Quality Study II (TexAQS). Ozone, a primary focus of the measurements, was above 80 ppb during 3 days and above 75 ppb during additional 8 days in summer 2006, suggestive of possible violations of the ozone National Ambient Air Quality Standard (NAAQS) in this area. In concordance with other air quality measurements during the TexAQS II, elevated ozone mixing ratios coincided with northerly flows during days after cold front passages. Ozone background during these days was as high as 80 ppb, whereas southerly air flows generally provided for an ozone background lower than 40 ppb. Back trajectory analysis shows that local ozone mixing ratios can also be strongly affected by the Houston urban pollution plume, leading to late afternoon ozone increases of as high as 50 ppb above background under favorable transport conditions. The trajectory analysis also shows that ozone background increases steadily the longer a southern air mass resides over Texas after entering from the Gulf of Mexico. In light of these and other TexAQS findings, it appears that ozone air quality is affected throughout east Texas by both long-range and regional ozone transport, and that improvements therefore will require at least a regionally oriented instead of the current locally oriented ozone precursor reduction policies.     

Development of a Speciated,Hourly, and Gridded Air Pollutants Emission Modeling System—A Case Study on the Precursors of Photochemical Smog in the Seoul Metropolitan Area,Korea

ABSTRACT

A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO₂) and ozone (O₃) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas.

The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO₂, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO₂ and O₃ concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.     

Measurements of ozone and nonmethane hydrocarbons at Chichi-jima island,a remote island in the western Pacific: long-range transport of polluted air from the Pacific rim region

Chichi-jima island is located in the Pacific about 1000 km from the Japanese main island and is an ideal remote observatory from which to assess the long-range transport of polluted air from East Asia. The ozone concentration was measured from August 1997 to August 1998. Owing to the air mass change, the seasonal variation of ozone shows a distinct character: low concentration (about 13 ppbv) for the maritime air mass during the summer, and high concentration (about 40 ppbv) for the continental air mass during the winter. To assess the contribution of the long-range transport of polluted air during winter, nonmethane hydrocarbons were also measured in December 1999. Using backward trajectory analysis, the transport time of the air mass from the source area in the Pacific rim region was calculated for each sample. The concentration of hydrocarbons shows a clear negative correlation against the transport time. This analysis clearly shows the transport of polluted air, emitted in East Asia, to the Pacific during the winter. The plots of suitable hydrocarbon pairs showed that the decrease of hydrocarbon concentrations during winter is mainly caused by the mixing with clean background air.     

The influence of south foehn on the ozone mixing ratios at the high alpine site Arosa

Within 2 years of trace gas measurements performed at Arosa (Switzerland, 2030 m above sea level), enhanced ozone mixing ratios were observed during south foehn events during summer and spring (5–10 ppb above the median value). The enhancements can be traced back to ozone produced in the strongly industrialized Po basin as confirmed by various analyses. Backward trajectories clearly show advection from this region during foehn. NO_y versus O₃ correlation and comparison of O₃ mixing ratios between Arosa and Mt. Cimone (Italy, 2165 m asl) suggest that ozone is the result of recent photochemical production (+5.6 ppb on average), either directly formed during the transport or via mixing of air processed in the Po basin boundary layer. The absence of a correlation between air parcel residence times over Europe and ozone mixing ratios at Arosa during foehn events is in contrast to a previous analysis, which suggested such correlation without reference to the origin of the air. In the case of south foehn, the continental scale influence of pollutants emission on ozone at Arosa appears to be far less important than the direct influence of the Po basin emissions. In contrast, winter time displays a different situation, with mean ozone reductions of about 4 ppb for air parcels passing the Po basin, probably caused by mixing with ozone-poor air from the Po basin boundary layer.     

Surface ozone at the Swiss Alpine site Arosa: the hemispheric background and the influence of large-scale anthropogenic emissions

An innovative and effective method using isentropic trajectory analysis based on the residence time of air masses over the polluted region of Europe was successfully applied to categorize surface ozone amounts at Arosa, Switzerland during 1996–1997. The “European representative” background ozone seasonal cycle at Arosa is associated with long-range transport of North Atlantic air masses, and displays the spring maximum–summer minimum with an annual average of 35 ppb. The photochemical ozone production due to the intense large-scale anthropogenic emission over Europe is estimated as high as 20 ppb in summer, whereas it is insignificant in winter. European sources contribute an annual net ozone production of 9–12 ppb at Arosa. Comparison with the selected regional representative site in Western Europe shows similar results indicating that the categorized ozone data at Arosa by this technique could be regarded as a representative for northern hemispheric mid-latitudes.     

Origin of polluted air masses in the Alps. An overview and first results for MONARPOP

The contribution of ZAMG to MONAROP consists of special weather forecasts to control the SOCs sampling procedure and of the analysis of the specific transport processes for SOCs, which is still in progress.In this paper, air pollutant transport into the Alps is demonstrated by examples of inorganic pollutants: Measurements of NO_x and ozone provide evidence for air pollutant transport by local wind systems (valley and slope winds), especially at low elevated sites of the Alps. In addition, trajectory analyses for the high elevation sites demonstrate the importance of large scale synoptic air pollutant transport. The effects of these transport processes with different spatial and temporal scales are governed by the physical and chemical properties of the particular pollutant.First results for the high alpine MONARPOP stations show that air masses from east Europe influence mostly Sonnblick (Austria), whereas the influence of the Po basin is strongest at Weissfluhjoch (Switzerland).     

Codependencies of Reactive Air Toxic and Criteria Pollutants on Emission Reductions

Abstract

It is important to understand the effects of emission controls on concentrations of ozone, fine particulate matter (PM_2.5), and hazardous air pollutants (HAPs) simultaneously, to evaluate the full range of health, ecosystem, and economic effects. Until recently, the capability to simultaneously evaluate interrelated atmospheric pollutants (“one atmosphere” analysis) was unavailable to air quality managers. In this work, we use an air quality model to examine the potential effect of three emission reductions on concentrations of ozone, PM_2.5, and four important HAPs (formaldehyde, acetaldehyde, acrolein, and benzene) over a domain centered on Philadelphia for 12-day episodes in July and January 2001. Although NO_x controls are predicted to benefit PM_2.5 concentrations and sometimes benefit ozone, they have only a small effect on formaldehyde, slightly increase acetaldehyde and acrolein, and have no effect on benzene in the July episode. Concentrations of all pollutants except benzene increase slightly with NO_x controls in the January simulation. Volatile organic compound controls alone are found to have a small effect on ozone and PM_2.5, a less than linear effect on decreasing aldehydes, and an approximately linear effect on acrolein and benzene in summer, but a slightly larger than linear effect on aldehydes and acrolein in winter. These simulations indicate the difficulty in assessing how toxic air pollutants might respond to emission reductions aimed at decreasing criteria pollutants such as ozone and PM_2.5.     

Codependencies of reactive air toxic and criteria pollutants on emission reductions

It is important to understand the effects of emission controls on concentrations of ozone, fine particulate matter (PM2.5), and hazardous air pollutants (HAPs) simultaneously, to evaluate the full range of health, ecosystem, and economic effects. Until recently, the capability to simultaneously evaluate interrelated atmospheric pollutants ("one atmosphere" analysis) was unavailable to air quality managers. In this work, we use an air quality model to examine the potential effect of three emission reductions on concentrations of ozone, PM2.5, and four important HAPs (formaldehyde, acetaldehyde, acrolein, and benzene) over a domain centered on Philadelphia for 12-day episodes in July and January 2001. Although NO(x) controls are predicted to benefit PM2.5 concentrations and sometimes benefit ozone, they have only a small effect on formaldehyde, slightly increase acetaldehyde and acrolein, and have no effect on benzene in the July episode. Concentrations of all pollutants except benzene increase slightly with NO(x) controls in the January simulation. Volatile organic compound controls alone are found to have a small effect on ozone and PM2.5, a less than linear effect on decreasing aldehydes, and an approximately linear effect on acrolein and benzene in summer, but a slightly larger than linear effect on aldehydes and acrolein in winter. These simulations indicate the difficulty in assessing how toxic air pollutants might respond to emission reductions aimed at decreasing criteria pollutants such as ozone and PM2.5.     

Integrated assessment modeling of atmospheric pollutants in the Southern Appalachian Mountains. Part I: hourly and seasonal ozone

Recently, a comprehensive air quality modeling system was developed as part of the Southern Appalachians Mountains Initiative (SAMI) with the ability to simulate meteorology, emissions, ozone, size- and composition-resolved particulate matter, and pollutant deposition fluxes. As part of SAMI, the RAMS/EMS-95/URM-1ATM modeling system was used to evaluate potential emission control strategies to reduce atmospheric pollutant levels at Class I areas located in the Southern Appalachians Mountains. This article discusses the details of the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. The daily mean normalized bias and error for 1-hr and 8-hr ozone were within U.S. Environment Protection Agency guidance criteria for urban-scale modeling. The model typically showed a systematic overestimation for low ozone levels and an underestimation for high levels. Because SAMI was primarily interested in simulating the growing season ozone levels in Class I areas, daily and seasonal cumulative ozone exposure, as characterized by the W126 index, were also evaluated. The daily ozone W126 performance was not as good as the hourly ozone performance; however, the seasonal ozone W126 scaled up from daily values was within 17% of the observations at two typical Class I areas of the SAMI region. The overall ozone performance of the model was deemed acceptable for the purposes of SAMI's assessment.     

Integrated Assessment Modeling of Atmospheric Pollutants in the Southern Appalachian Mountains. Part I: Hourly and Seasonal Ozone

Abstract

Recently, a comprehensive air quality modeling system was developed as part of the Southern Appalachians Mountains Initiative (SAMI) with the ability to simulate meteorology, emissions, ozone, size- and composition-resolved particulate matter, and pollutant deposition fluxes. As part of SAMI, the RAMS/EMS-95/URM-1ATM modeling system was used to evaluate potential emission control strategies to reduce atmospheric pollutant levels at Class I areas located in the Southern Appalachians Mountains. This article discusses the details of the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. The daily mean normalized bias and error for 1-hr and 8-hr ozone were within U.S. Environment Protection Agency guidance criteria for urban-scale modeling. The model typically showed a systematic overestimation for low ozone levels and an underestimation for high levels. Because SAMI was primarily interested in simulating the growing season ozone levels in Class I areas, daily and seasonal cumulative ozone exposure, as characterized by the W126 index, were also evaluated. The daily ozone W126 performance was not as good as the hourly ozone performance; however, the seasonal ozone W126 scaled up from daily values was within 17% of the observations at two typical Class I areas of the SAMI region. The overall ozone performance of the model was deemed acceptable for the purposes of SAMI’s assessment.     

High ozone levels in the northeast of Portugal: Analysis and characterization

Each summer period extremely high ozone levels are registered at the rural background station of Lamas d'Olo, located in the Northeast of Portugal. In average, 30% of the total alert threshold registered in Portugal is detected at this site. The main purpose of this study is to characterize the atmospheric conditions that lead to the ozone-rich episodes at this site. Synoptic patterns anomalies and back trajectories cluster analysis were performed, for the period between 2004 and 2007, considering 76 days when ozone maximum hourly concentrations were above 200 μg m^?3. The obtained atmospheric anomaly fields suggested that a positive temperature anomaly is visible above the Iberian Peninsula. A strong wind flow pattern from NE is observable in the North of Portugal and Galicia, in Spain. These two features may lead to an enhancement of the photochemical production and to the transport of pollutants from Spain to Portugal. In addition, the 3D mean back trajectories associated to the ozone episode days were analysed. A clustering method has been applied to the obtained back trajectories. Four main clusters of ozone-rich episodes were identified, with different frequencies of occurrence: north-westerly flows (11%); north-easterly flows (45%), southern flow (4%) and westerly flows (40%). Both analyses highlight the NE flow as a dominant pattern over the North of Portugal during summer. The analysis of the ozone concentrations for each selected cluster indicates that this northeast circulation pattern, together with the southern flow, are responsible for the highest ozone peak episodes. This also suggests that long-range transport of atmospheric pollutants is the main contributor to the ozone levels registered at Lamas d'Olo. This is also highlighted by the correlation of the ozone time-series with the meteorological parameters analysed in the frequency domain.     

Air quality impacts of distributed energy resources implemented in the northeastern United States

Emissions from the potential installation of distributed energy resources (DER) in the place of current utility-scale power generators have been introduced into an emissions inventory of the northeastern United States. A methodology for predicting future market penetration of DER that considers economics and emission factors was used to estimate the most likely implementation of DER. The methodology results in spatially and temporally resolved emission profiles of criteria pollutants that are subsequently introduced into a detailed atmospheric chemistry and transport model of the region. The DER technology determined by the methodology includes 62% reciprocating engines, 34% gas turbines, and 4% fuel cells and other emerging technologies. The introduction of DER leads to retirement of 2625 MW of existing power plants for which emissions are removed from the inventory. The air quality model predicts maximum differences in air pollutant concentrations that are located downwind from the central power plants that were removed from the domain. Maximum decreases in hourly peak ozone concentrations due to DER use are 10 ppb and are located over the state of New Jersey. Maximum decreases in 24-hr average fine particulate matter (PM2.5) concentrations reach 3 microg/m3 and are located off the coast of New Jersey and New York. The main contribution to decreased PM2.5 is the reduction of sulfate levels due to significant reductions in direct emissions of sulfur oxides (SO(x)) from the DER compared with the central power plants removed. The scenario presented here represents an accelerated DER penetration case with aggressive emission reductions due to removal of highly emitting power plants. Such scenario provides an upper bound for air quality benefits of DER implementation scenarios.     

Air Quality Impacts of Distributed Energy Resources Implemented in the Northeastern United States

Abstract

Emissions from the potential installation of distributed energy resources (DER) in the place of current utility-scale power generators have been introduced into an emissions inventory of the northeastern United States. A methodology for predicting future market penetration of DER that considers economics and emission factors was used to estimate the most likely implementation of DER. The methodology results in spatially and temporally resolved emission profiles of criteria pollutants that are subsequently introduced into a detailed atmospheric chemistry and transport model of the region. The DER technology determined by the methodology includes 62% reciprocating engines, 34% gas turbines, and 4% fuel cells and other emerging technologies. The introduction of DER leads to retirement of 2625 MW of existing power plants for which emissions are removed from the inventory. The air quality model predicts maximum differences in air pollutant concentrations that are located downwind from the central power plants that were removed from the domain. Maximum decreases in hourly peak ozone concentrations due to DER use are 10 ppb and are located over the state of New Jersey. Maximum decreases in 24-hr average fine particulate matter (PM_2.5) concentrations reach 3 μg/m3 and are located off the coast of New Jersey and New York. The main contribution to decreased PM_2.5 is the reduction of sulfate levels due to significant reductions in direct emissions of sulfur oxides (SO_x) from the DER compared with the central power plants removed. The scenario presented here represents an accelerated DER penetration case with aggressive emission reductions due to removal of highly emitting power plants. Such scenario provides an upper bound for air quality benefits of DER implementation scenarios.     

Increase in summer European ozone amounts due to climate change

The local and regional distribution of pollutants is significantly influenced by weather patterns and variability along with the spatial patterns of emissions. Therefore, climatic changes which affect local meteorological conditions can alter air quality. We use the regional air quality model CHIMERE driven by meteorological fields from regional climate change simulations to investigate changes in summer ozone mixing ratios over Europe under increased greenhouse gas (GHG) forcing. Using three 30-year simulation periods, we find that daily peak ozone amounts as well as average ozone concentrations substantially increase during summer in future climate conditions. This is mostly due to higher temperatures and reduced cloudiness and precipitation over Europe and it leads to a higher number of ozone events exceeding information and warning thresholds. Our results show a pronounced regional variability, with the largest effects of climate change on ozone concentrations occurring over England, Belgium, Germany and France. The temperature-driven increase in biogenic emissions appears to enhance the ozone production and isoprene was identified as the most important chemical factor in the ozone sensitivity. We also find that summer ozone levels in future climate projections are similar to those found during the exceptionally warm and dry European summer of 2003. Our simulations suggest that in future climate conditions summer ozone might pose a much more serious threat to human health, agriculture and natural ecosystems in Europe, so that the effects of climate trends on pollutant amounts should be considered in future emission control measures.     

Expected ozone benefits of reducing nitrogen oxide (NOx) emissions from coal-fired electricity generating units in the eastern United States

On hot summer days in the eastern United States, electricity demand rises, mainly because of increased use of air conditioning. Power plants must provide this additional energy, emitting additional pollutants when meteorological conditions are primed for poor air quality. To evaluate the impact of summertime NO_x emissions from coal-fired electricity generating units (EGUs) on surface ozone formation, we performed a series of sensitivity modeling forecast scenarios utilizing EPA 2018 version 6.0 emissions (2011 base year) and CMAQ v5.0.2. Coal-fired EGU NO_x emissions were adjusted to match the lowest NO_x rates observed during the ozone seasons (April 1–October 31) of 2005–2012 (Scenario A), where ozone decreased by 3–4 ppb in affected areas. When compared to the highest emissions rates during the same time period (Scenario B), ozone increased ～4–7 ppb. NO_x emission rates adjusted to match the observed rates from 2011 (Scenario C) increased ozone by ～4–5 ppb. Finally in Scenario D, the impact of additional NO_x reductions was determined by assuming installation of selective catalytic reduction (SCR) controls on all units lacking postcombustion controls; this decreased ozone by an additional 2–4 ppb relative to Scenario A. Following the announcement of a stricter 8-hour ozone standard, this analysis outlines a strategy that would help bring coastal areas in the mid-Atlantic region closer to attainment, and would also provide profound benefits for upwind states where most of the regional EGU NO_x originates, even if additional capital investments are not made (Scenario A).

Implications: With the 8-hr maximum ozone National Ambient Air Quality Standard (NAAQS) decreasing from 75 to 70 ppb, modeling results indicate that use of postcombustion controls on coal-fired power plants in 2018 could help keep regions in attainment. By operating already existing nitrogen oxide (NO_x) removal devices to their full potential, ozone could be significantly curtailed, achieving ozone reductions by up to 5 ppb in areas around the source of emission and immediately downwind. Ozone improvements are also significant (1–2 ppb) for areas affected by cross-state transport, especially Mid-Atlantic coast regions that had struggled to meet the 75 ppb standard.     

Evidence of enhanced atmospheric ammoniacal nitrogen in Hells Canyon national recreation area: implications for natural and cultural resources

Agriculture releases copious fertilizing pollutants to air sheds and waterways of the northwestern United States. To evaluate threats to natural resources and historic rock paintings in remote Hells Canyon, Oregon and Idaho, deposition of ammonia (NH3), nitrogen oxides (NOx), sulfur dioxide (SO2), and hydrogen sulfide (H2S) at five stations along 60 km of the Snake River valley floor were passively sampled from July 2002 through June 2003, and ozone data and particulate chemistry were obtained from the Interagency Monitoring of Protected Visual Environments (IMPROVE) station at Hells Canyon. NH3 concentrations were high; biweekly averages peaked at 5-19 ppb in spring and summer and the nutrient-laden Snake River is a likely source. Fine particulate ammonium nitrate (NH4NO3) averaged 2.6 microg/m3 during the 20% of worst visibility days with winter drainage of air masses from the Snake River Basin and possibly long distance transport from southern California. Other pollutants were within background ranges. NH3 is corrosive to clay-based pictographs; nitrogen deposition can alter natural biotic communities and terrestrial ecosystem processes at levels reported here.     

Natural emissions for regional modeling of background ozone and particulate matter and impacts on emissions control strategies

Natural emissions adopted in current regional air quality modeling are updated to better describe natural background ozone and PM concentrations for North America. The revised natural emissions include organosulfur from the ocean, NO from lightning, sea salt, biogenic secondary organic aerosol (SOA) precursors, and pre-industrial levels of background methane. The model algorithm for SOA formation was also revised. Natural background ozone concentrations increase by up to 4 ppb in annual average over the southeastern US and Gulf of Mexico due to added NO from lightning while the revised biogenic emissions produced less ozone in the central and western US. Natural PM_2.5 concentrations generally increased with the revised natural emissions. Future year (2018) simulations were conducted for several anthropogenic emission reduction scenarios to assess the impact of the revised natural emissions on anthropogenic emission control strategies. Overall, the revised natural emissions did not significantly alter the ozone responses to the emissions reductions in 2018. With revised natural emissions, ozone concentrations were slightly less sensitive to reducing NOx in the southeastern US than with the current natural emissions due to higher NO from lightning. The revised natural emissions have little impact on modeled PM_2.5 responses to anthropogenic emission reductions. However, there are substantial uncertainties in current representations of natural sources in air quality models and we recommend that further study is needed to refine these representations.