Atmospheric composition change – global and regional air quality

Air quality transcends all scales with in the atmosphere from the local to the global with handovers and feedbacks at each scale interaction. Air quality has manifold effects on health, ecosystems, heritage and climate. In this review the state of scientific understanding in relation to global and regional air quality is outlined. The review discusses air quality, in terms of emissions, processing and transport of trace gases and aerosols. New insights into the characterization of both natural and anthropogenic emissions are reviewed looking at both natural (e.g. dust and lightning) as well as plant emissions. Trends in anthropogenic emissions both by region and globally are discussed as well as biomass burning emissions. In terms of chemical processing the major air quality elements of ozone, non-methane hydrocarbons, nitrogen oxides and aerosols are covered. A number of topics are presented as a way of integrating the process view into the atmospheric context; these include the atmospheric oxidation efficiency, halogen and HO_x chemistry, nighttime chemistry, tropical chemistry, heat waves, megacities, biomass burning and the regional hot spot of the Mediterranean. New findings with respect to the transport of pollutants across the scales are discussed, in particular the move to quantify the impact of long-range transport on regional air quality. Gaps and research questions that remain intractable are identified. The review concludes with a focus of research and policy questions for the coming decade. In particular, the policy challenges for concerted air quality and climate change policy (co-benefit) are discussed.     

Extensive aerosol optical properties and aerosol mass related measurements during TRAMP/TexAQS 2006 – Implications for PM compliance and planning

Extensive aerosol optical properties, particle size distributions, and Aerodyne quadrupole aerosol mass spectrometer measurements collected during TRAMP/TexAQS 2006 were examined in light of collocated meteorological and chemical measurements. Much of the evident variability in the observed aerosol-related air quality is due to changing synoptic meteorological situations that direct emissions from various sources to the TRAMP site near the center of the Houston-Galveston-Brazoria (HGB) metropolitan area. In this study, five distinct long-term periods have been identified. During each of these periods, observed aerosol properties have implications that are of interest to environmental quality management agencies. During three of the periods, long range transport (LRT), both intra-continental and intercontinental, appears to have played an important role in producing the observed aerosol. During late August 2006, southerly winds brought super-micron Saharan dust and sea salt to the HGB area, adding mass to fine particulate matter (PM_2.5) measurements, but apparently not affecting secondary particle growth or gas-phase air pollution. A second type of LRT was associated with northerly winds in early September 2006 and with increased ozone and sub-micron particulate matter in the HGB area. Later in the study, LRT of emissions from wildfires appeared to increase the abundance of absorbing aerosols (and carbon monoxide and other chemical tracers) in the HGB area. However, the greatest impacts on Houston PM_2.5 air quality are caused by periods with low-wind-speed sea breeze circulation or winds that directly transport pollutants from major industrial areas, i.e., the Houston Ship Channel, into the city center.     

The Evolution of Visibility Deterioration and Aerosol Spectra in the St. Louis Urban Plume

Under the auspices of Project METROMEX, studies of visibility de-teoration downwind of St. Louis were conducted during July-August 1974-1975. Estimates of horizontal visual range, standard meteorological data, and aerosol characteristics within the mixing layer were acquired upwind, over, and downwind of the metropolitan area by means of airborne transects. Aerosol number, surface, and volume distributions for particles between 0.025-2.5 µm were generated from the airborne measurement of Aitken nucleus concentrations, cloud condensation nuclei, and aerosols detected in situ with optical probes. Visibility reduction amounting to 50% of prevailing regional upwind visibilities consistently occurs at a distance corresponding to 2-3 hours travel time downwind for an air parcel moving with the mean transport wind. The regions of visibility minimum do not coincide with locations of maximum Aitken nucleus concentrations, but rather correspond in space and time to increased values of cloud condensation nuclei and increased numbers of particles in the 0.1-2.5 µm diameter range. Comparisons of observed aerosol evolution with similar laboratory studies suggest that most of the light scattering aerosols are of secondary origin.     

Radiative forcing from household fuel burning in Asia

Household fuel use in developing countries, particularly as biomass and coal, is a major source of carbonaceous aerosols and other air pollutants affecting health and climate. Using state-of-the-art emission inventories, a global three-dimensional photochemical tracer/transport model of the troposphere, and a global radiative transfer model based on methods presented in the latest IPCC Assessment Report (2007-AR4), we estimate the radiative forcing (RF) attributable to household fuel combustion in Asia in terms of current global annual-mean RF and future global integrated RF for a one-year pulse of emissions (2000) over two time horizons (100 and 20 years). Despite the significant emissions of black carbon (BC) aerosols, these estimates indicate that shorter-lived (non-Kyoto) air pollutants from household fuel use in the region overall seem to exert a small net negative RF because of the strong influence of reflective aerosols. There are, however, major uncertainties in emission estimates for solid fuel burning, and about the sustainability of household fuel wood harvesting in Asia (the carbon neutrality of harvesting). In addition, there is still substantial uncertainty associated with the BC radiative forcing. As a result we find that the sign of the RF from household biomass burning in the region cannot be established. While recognizing the value of integrating climate change and air pollution policies, we are concerned that for a ‘Kyoto style’ post-Kyoto treaty (with global cap-and-trade and the Global Warming Potential as the metric) expanding the basket of components with a selection of short-lived species without also including the wider range of co-emitted species may lead to unintended consequences for global-scale climate. Additional measurement, modelling, and policy research is urgently needed to reduce the uncertainties so that the net impact on climate of emissions and mitigation measures in this sector can be accurately assessed.     

Local Arctic air pollution: Sources and impacts

Local emissions of Arctic air pollutants and their impacts on climate, ecosystems and health are poorly understood. Future increases due to Arctic warming or economic drivers may put additional pressures on the fragile Arctic environment already affected by mid-latitude air pollution. Aircraft data were collected, for the first time, downwind of shipping and petroleum extraction facilities in the European Arctic. Data analysis reveals discrepancies compared to commonly used emission inventories, highlighting missing emissions (e.g. drilling rigs) and the intermittent nature of certain emissions (e.g. flaring, shipping). Present-day shipping/petroleum extraction emissions already appear to be impacting pollutant (ozone, aerosols) levels along the Norwegian coast and are estimated to cool and warm the Arctic climate, respectively. Future increases in shipping may lead to short-term (long-term) warming (cooling) due to reduced sulphur (CO₂) emissions, and be detrimental to regional air quality (ozone). Further quantification of local Arctic emission impacts is needed.     

An online coupled meteorological and air quality modeling study of the effect of complex terrain on the regional transport and transformation of air pollutants over the Western United States

One of the most prominent of characteristics of the western United States that affects its meteorology is the complexity of its mountainous terrain. The meteorological Mesoscale Model, version 5 with Chemistry (MM5-Chem), an online-coupled atmospheric chemistry model, was used to investigate the effect of this terrain on a high air pollution event in the free troposphere. The simulations were evaluated by comparisons with data from the North American Regional Reanalysis (NARR). Complex terrain was shown to have an important influence on the vertical transport of air pollutants on the regional scale; emissions from ground level were vertically mixed as high as 5 km above sea surface level for the wintertime conditions simulated. The simulations showed that the vertical transport of emissions from the Earth's surface could have a more significant effect on mid and upper level chemical concentrations than chemical production. The vertical transport was caused predominately by terrain forced flow over the mountains’ ridge-line and the terrain forced flow was affected by the mountain peak height and the complexity of the terrain downwind.     

Air pollution,greenhouse gases and climate change: Global and regional perspectives

Greenhouse gases (GHGs) warm the surface and the atmosphere with significant implications for rainfall, retreat of glaciers and sea ice, sea level, among other factors. About 30 years ago, it was recognized that the increase in tropospheric ozone from air pollution (NO_x, CO and others) is an important greenhouse forcing term. In addition, the recognition of chlorofluorocarbons (CFCs) on stratospheric ozone and its climate effects linked chemistry and climate strongly. What is less recognized, however, is a comparably major global problem dealing with air pollution. Until about ten years ago, air pollution was thought to be just an urban or a local problem. But new data have revealed that air pollution is transported across continents and ocean basins due to fast long-range transport, resulting in trans-oceanic and trans-continental plumes of atmospheric brown clouds (ABCs) containing sub micron size particles, i.e., aerosols. ABCs intercept sunlight by absorbing as well as reflecting it, both of which lead to a large surface dimming. The dimming effect is enhanced further because aerosols may nucleate more cloud droplets, which makes the clouds reflect more solar radiation. The dimming has a surface cooling effect and decreases evaporation of moisture from the surface, thus slows down the hydrological cycle. On the other hand, absorption of solar radiation by black carbon and some organics increase atmospheric heating and tend to amplify greenhouse warming of the atmosphere.ABCs are concentrated in regional and mega-city hot spots. Long-range transport from these hot spots causes widespread plumes over the adjacent oceans. Such a pattern of regionally concentrated surface dimming and atmospheric solar heating, accompanied by widespread dimming over the oceans, gives rise to large regional effects. Only during the last decade, we have begun to comprehend the surprisingly large regional impacts. In S. Asia and N. Africa, the large north-south gradient in the ABC dimming has altered both the north-south gradients in sea surface temperatures and land–ocean contrast in surface temperatures, which in turn slow down the monsoon circulation and decrease rainfall over the continents. On the other hand, heating by black carbon warms the atmosphere at elevated levels from 2 to 6 km, where most tropical glaciers are located, thus strengthening the effect of GHGs on retreat of snow packs and glaciers in the Hindu Kush-Himalaya-Tibetan glaciers.Globally, the surface cooling effect of ABCs may have masked as much 47% of the global warming by greenhouse gases, with an uncertainty range of 20–80%. This presents a dilemma since efforts to curb air pollution may unmask the ABC cooling effect and enhance the surface warming. Thus efforts to reduce GHGs and air pollution should be done under one common framework. The uncertainties in our understanding of the ABC effects are large, but we are discovering new ways in which human activities are changing the climate and the environment.     

Elemental composition of aerosol in the Nam Co region,Tibetan Plateau,during summer monsoon season

In order to investigate the chemical characteristics of atmospheric aerosols in a remote region of the Tibetan Plateau, total suspended particles were collected continuously at the Nam Co Comprehensive Observation and Research Station from July to October 2005. The PIXE analytical results showed that Si, Ca, Fe, Al, K, and S were the major components of aerosols, ranging from 82 (K)–550 (Si) ng m⁻³. The mean elemental concentrations were comparable with those from other remote sites and significantly lower than those from megacities (e.g. Beijing). The very low presence of anthropogenic elements demonstrates that the Nam Co region is an ideal background site for atmospheric monitoring. Crustal enrichment factor (EF) calculation indicated that several anthropogenic heavy metals (Cr, Ni, Cu, Zn, As) are transported long distances atmospherically. The backward air mass trajectory analysis suggests that South Asia may be the source region of those pollutants.     

Review of Singapore's air quality and greenhouse gas emissions: current situation and opportunities

Singapore has many environmental accomplishments to its credit. Accessible data on air quality indicates that all criteria pollutants satisfy both U.S. Environmental Protection Agency (EPA) and World Health Organization (WHO) air quality standards and guidelines, respectively. The exception is PM2.5 (particles with an aerodynamic diameter < or = 2.5 microm), which is not currently considered a criteria pollutant in Singapore but may potentially be the major local air pollution problem and cause for health concern. Levels of other airborne pollutants as well as their physical and chemical processes associated with local formation, transformation, dispersion, and deposition are not known. According to available emission inventories, Singapore contribution to the total atmospheric pollution and carbon budget at the regional and global scales is small. Emissions per unit gross domestic product (GDP) are low compared with other countries, although Singapore's per-capita GDP and per-capita emissions are among the highest in the world. Some information is available on health effects, but the impacts on the ecosystem and the complex interactions of air pollution and climate change at a regional level are also unknown. This article reviews existing available information on atmospheric pollution and greenhouse gas emissions and proposes a multipollutant approach to greenhouse gas mitigation and local air quality. Singapore, by reducing its per-capita emissions, increasing the availability of information (e.g., through regularly publishing hourly and/or daily PM2.5 concentrations) and developing a research agenda in this area, would likely be seen to be a model of a high-density, livable, and sustainable city in Southeast Asia and other tropical regions worldwide.     

Contemporary threats and air pollution

It is now well understood that air pollution produces significant adverse health effects in the general public and over the past 60 years, there have been on-going efforts to reduce the emitted pollutants and their resulting health effects. There are now shifting patterns of industrialization with many heavily polluting industries moving from developed countries with increasingly stringent air quality standards to the developing world. However, even in decreasing concentrations of pollutants, health effects remain important possibly as a result of changes in the nature of the pollutants as new chemicals are produced and as other causes of mortality and morbidity are reduced. In addition, there is now the potential for deliberate introduction of toxic air pollutants by local armed conflicts and terrorists. Thus, there are new challenges to understand the role of the atmospheric environment on public health in this time of changing economic and demographic conditions overlaid with the willingness to indirectly attack governments and other established entities through direct attacks on the general public.     

Optical properties of tropospheric aerosols based on measurements of lidar,sun-photometer,and visibility at Chung-Li (25°N, 121°E)

We have used lidar, sun-photometer, and the visibility measurements to investigate the optical properties of aerosols in the lower air. The observations were performed at Chung-Li (25°N, 121°E) during the period of February 2002–May 2004. Combined data indicate that 40–50% of total extinction in the column air contributed by aerosols in 1–5 km. Seasonally, spring time extinction is higher than other seasons. However, the summer extinction is the highest below about 2 km. Sources for aerosols are determined by using satellite imageries and back trajectories. Aerosols backscattering ratio and depolarization ratio are then categorized based on their sources. We found that the largest optical thickness is biomass burning aerosols originated in Southeast Asia. The aerosols generated from Northern China transported by the high-pressure system in spring are usually dust with depolarization ratios in the range of 0.1–0.3, but varying backscattering coefficients. The aerosols optical characteristics will be useful for future understanding about their environmental and climate effects.     

The impacts of combustion emissions on air quality and climate – From coal to biofuels and beyond

Combustion processes have inherent characteristics that lead to the release in the environment of both gaseous and particulate pollutants that have primary and secondary impacts on air quality, human health, and climate. The emissions from the combustion of fossil fuels and biofuels and their atmospheric impacts are reviewed here with attention given to the emissions of the currently regulated pollutant gasses, primary aerosols, and secondary aerosol precursors as well as the emissions of non-regulated pollutants. Fuels ranging from coal, petroleum, liquefied petroleum gas (LPG), natural gas, as well as the biofuels; ethanol, methanol, methyl tertiary-butyl ether (MTBE), ethyl tertiary-butyl ether (ETBE), and biodiesel, are discussed in terms of the known air quality and climate impacts of the currently regulated pollutants. The potential importance of the non-regulated emissions of both gasses and aerosols in air quality issues and climate is also discussed with principal focus on aldehydes and other oxygenated organics, polycyclic aromatic hydrocarbons (PAHs), and nitrated organics. The connection between air quality and climate change is also addressed with attention given to ozone and aerosols as potentially important greenhouse species.     

The effects of roadside structures on the transport and dispersion of ultrafine particles from highways

Understanding local-scale transport and dispersion of pollutants emitted from traffic sources is important for urban planning and air quality assessments. Predicting pollutant concentration patterns in complex environments depends on accurate representations of local features (e.g., noise barriers, trees, buildings) affecting near-field air flows. This study examined the effects of roadside barriers on the flow patterns and dispersion of pollutants from a high-traffic highway in Raleigh, North Carolina, USA. The effects of the structures were analyzed using the Quick Urban & Industrial Complex (QUIC) model, an empirically based diagnostic tool which simulates fine-scale wind field and dispersion patterns around obstacles. Model simulations were compared with the spatial distributions of ultrafine particles (UFP) from vehicular emissions measured using a passenger van equipped with a Differential Mobility Analyzer/Condensation Particle Counter. The field site allowed for an evaluation of pollutant concentrations in open terrain, with a noise barrier present near the road, and with a noise barrier and vegetation present near the road.Results indicated that air pollutant concentrations near the road were generally higher in open terrain situations with no barriers present; however, concentrations for this case decreased faster with distance than when roadside barriers were present. The presence of a noise barrier and vegetation resulted in the lowest downwind pollutant concentrations, indicating that the plume under this condition was relatively uniform and vertically well-mixed. Comparison of the QUIC model with the mobile UFP measurements indicated that QUIC reasonably represented pollutant transport and dispersion for each of the study configurations.     

Study on the formation and transport of ozone in relation to the air quality management and vegetation protection in Tenerife (Canary Islands)

An experimental study on the formation and transport of ozone in ambient air was performed in Tenerife (Canary Islands) in order to investigate the processes affecting ozone levels and air quality. The special features of Tenerife (prevalence of the trade wind pattern (NE), orography and the specific location of the local ozone sources) permit to quantify the role of the ‘long-range transport from northern latitudes' versus the ‘formation and transport of ozone downwind of the main urban areas' of Tenerife. Levels of O₃, NO₂ and O_X were monitored in different types of environments to achieve this purpose. The results showed that: (1) upwind of the urban areas ozone is mainly transported from the ocean by trade winds, (2) local ozone titration (by NO) and ozone replenishment from the ocean are the main causes of ozone variations in urban and suburban areas, and (3) photochemical ozone production occurs downwind of the urban areas. Photochemical production causes daylight O₃ and O_X levels downwind of urban areas to be frequently (60% and 35% days/year, respectively) higher than upwind of the urban sites (O₃ and O_X excess frequently in the range 5–20 ppbv). Due to the above processes, different daily ozone cycles occur in short distances (<30 km), with maximum O₃ levels during daylight or night depending on the site. Ozone phytotoxicity was assessed by calculating the AOT40 index upwind and downwind of the main urban areas. The critical value for the 5-day-AOT40 index was simultaneously exceeded at the two sites (few times/year) during long-range transport events. During the additional exceedances of the critical value downwind of the urban area, relatively high 5-day-AOT40 values were recorded upwind of the urban site. Thus, long-range transport from northern latitudes may produce relatively high 5-days-AOT40 levels in the oceanic boundary layer. These results are important for the protection of the large number of endemic plants in the Canaries. The conceptual model discussed in this study may be qualitatively applied to other islands which possess features similar to those of Tenerife.     

Field observations of regional and urban impacts on NO2, ozone,UVB, and nitrate radical production rates in the Phoenix air basin

In the May and June of 1998, field measurements were taken at a site near the Usery Pass Recreation Area, ∼27 miles from the downtown Phoenix area, overlooking Phoenix and Mesa, Arizona. This site was selected to examine the impacts of the Phoenix urban plume on the Usery Pass Recreation Area and surrounding regions. Data were obtained for ultraviolet-B (UVB) radiation, nitrogen dioxide (NO₂), peroxyacetyl nitrate (PAN), ozone (O₃), and carbon monoxide (CO). Nocturnal plumes of NO₂ (in tens of ppb), observed near midnight, were correlated with CO and anti-correlated with O₃. This behavior was consistent with the titration of locally generated NO by boundary layer O₃ to form the nighttime NO₂ plumes that were subsequently transported into the Usery Pass Recreation area. Nitrate radical (NO₃) production rates were calculated to be very high on the edges of these nocturnal plumes. Examination of O₃ and PAN data also indicates that Phoenix is being affected by long-range transport of pollutants from the Los Angeles to San Diego areas. A regional smoke episode was observed in May, accompanied by a decrease in UVB of factor of two and a decrease in O₃ and an increase in methyl chloride. Low level back trajectories and chemical evidence confirm that the smoke event originated in northern Mexico and that the reduced O₃ levels observed at Usery Pass could be partially due to reduced photolysis rates caused by carbonaceous soot aerosols transported in the smoke plume. The results are discussed with regard to potential effects of local pollution transport from the Phoenix air basin as well as an assessment of the contributions from long-range transport of pollutants to the background levels in the Phoenix-Usery Pass area.     

Observation of carbonaceous aerosols during 2006–2009 in Nyainqêntanglha Mountains and the implications for glaciers

Atmospheric carbonaceous aerosols were sampled discontinuously from July 2006 to December 2009 at Nam Co Comprehensive Observation and Research Station (NCOS) in the central Tibetan Plateau (TP). The mean daily concentration of carbonaceous aerosols increased from 268 to 330 ng?m^?3, and pollution episodes could significantly increase the mean level of carbonaceous aerosols in the total mass concentration. Organic carbon was the main component of carbonaceous aerosols at NCOS, and black carbon (BC) accounted for 5.8 %. Seven-day air masses backward trajectories calculated by the Hybrid Single-Particle Lagrangian Integrated Trajectory model and the aerosol optical depth distribution in the TP and South Asia both suggested that atmospheric pollutants emitted from Northern India and South Asia could penetrate into central TP by southwest winds. Due to the seasonal variations of emission sources and regional atmospheric conditions, calculated BC deposition flux in the nonmonsoon season was higher than that in the monsoon season. Increased BC concentration in snowpack in winter from 2007 to 2009 indicated that the atmospheric environment in central TP became more polluted and the influences from human activities have strengthened. Pollution episodes could significantly increase BC concentrations in the snowpack on a seasonal scale, which would furthermore affect the surface albedo.     

Shock Wave Cleaning of Air Filters

The trends in and relationships between ambient air concentrations of sulfur dioxide and sulfate aerosols at 48 urban sites and 27 nonurban sites throughout the U.S. between 1963 and 1972 have been analyzed. The substantial decreases in ambient SO₂ concentrations measured at urban sites in the eastern and midwestern U.S. are consistent with the corresponding reductions in local SO₂ emissions, but these decreases have been accompanied by only modest decreases in ambient sulfate concentrations. Large differences in the amounts of SO₂ emitted within individual air quality control regions are associated with much smaller differences in the corresponding ambient sulfate concentrations. Substantial changes in the patterns of SO₂ emissions between air quality regions result in essentially no differences between ambient sulfate concentrations in those air quality regions. Comparisons of several air quality regions in the eastern and western U.S. with similar SO₂ emission levels and patterns of emissions clearly demonstrates the higher ambient sulfate concentration levels in eastern air quality control regions. Relationships between SO₂, sulfates, and vanadium concentrations at eastern nonurban U.S. sites cannot be explained by local emission sources. These various observed results can be best explained by long distance sulfur oxide transport with chemical conversion of SO₂ to sulfates occurring over ranges of hundreds of kilometers. This conclusion has been suggested earlier and the present analysis strongly supports previous discussions. An impact of long range transport of sulfates is to emphasize the need for Consistent strategies for reduction of sulfur oxides throughout large geographical regions. Additions of large capacities involving elevated sources in mid-continental or western regions could result in significant increases in sulfate concentrations well downwind of such sources. Some of the types of research activities required to quantitate crucial experimental parameters are discussed.     

Trans-boundary air pollution over remote islands in Japan: observed data and estimates from a numerical model

Observations of air pollutants were conducted in remote Japanese islands (Oki Island and Okinawa Island) in early spring to clarify the extent of trans-boundary air pollution from the Asian continent. A three-dimensional Eulerian model calculation, which included parameters on emission, transport and transformation of sulfur oxides, nitrogen oxides and ammonia, was performed to compile sulfate isosurface concentrations over the observational sites. Concentrations of non-sea-salt sulfate (nss-SO₄²⁻) of greater than 10 μg m⁻³ were observed at Oki after the northeastward passage of low-pressure systems in the Sea of Japan. At these times, the weather showed a typical winter pattern and air pollutants over China were transported southeastward to Japan with the northwesterly wind. The model calculation reproduced the observed variations of nss-SO₄²⁻ concentration well, except for one case in which the model calculation could not reproduce the extremely low nss-SO₄²⁻ concentration observed on 8 March. In Hedo (Okinawa Island), we observed long-lasting (3 days) medium concentrations of nss-SO₄²⁻ (approximately 5 μg m⁻³). Although the model reproduced these observed medium concentrations well, in general the observed results were reproduced better for Oki than for Hedo. Under the synoptic weather conditions of early spring, high concentrations of nss-sulfate were sometimes transported to these remote Japanese islands from areas of continental Asia with a strong outflow of air pollutants.     

Spatial pattern of ozone injury in Aleppo pine related to air pollution dynamics in a coastal-mountain region of eastern Spain

In eastern Spain, studies combining the tracking and meso-scale circulations of air pollutants with the evaluation of their effects on plants have been undertaken since 1994. Meso-scale processes are very important from the point of view of how and where forest ecosystems are affected by point sources and regional air pollution in the Mediterranean area. The first results of these field surveys show that in 1994, 1995 and 1996, the distribution pattern of ozone visual injury (chlorotic mottle) in Pinus halepensis correlated with the penetration of pollutants transported by the sea-breeze into coastal valleys of Castellón (eastern Spain). In this tree species, longer needles are associated with higher chlorotic mottle, and ozone injury seems to be among the factors affecting needle retention and crown transparency.