Mercury pollution trends in subarctic lakes in the northern Swedish mountains

Despite many years of research about mercury pollution, data concerning high-latitude regions of Europe are limited, particularly studies of long-term temporal trends. It is not clear whether the mercury load at high latitudes follows the recent decreasing trends in European mercury emissions or whether the load is still high because of continuing global emissions. In this study we use sediments from 12 lakes, located above the Arctic Circle in the Swedish mountains, to assess the past and recent mercury pollution situation, especially for the last 200 y. The mercury load increased clearly in sediment deposited from the late 19th or early 20th century to a peak between 1960 and 1990. This peak represents an enrichment of 1.4 to 4.2 times over background concentrations. This enrichment is comparable with enrichments in sediments from lower latitudes as well as other Arctic regions. Since the 1990s mercury concentration has declined in 8 of the 12 lakes, i.e., similar to emission trends in Europe.     

Trends in on-road vehicle emissions and ambient air quality in Atlanta,Georgia, USA,from the late 1990s through 2009

On-road vehicle emissions of carbon monoxide (CO), nitrogen oxides (NO_x), and volatile organic compounds (VOCs) during 1995–2009 in the Atlanta Metropolitan Statistical Area were estimated using the Motor Vehicle Emission Simulator (MOVES) model and data from the National Emissions Inventories and the State of Georgia. Statistically significant downward trends (computed using the nonparametric Theil-Sen method) in annual on-road CO, NO_x, and VOC emissions of 6.1%, 3.3%, and 6.0% per year, respectively, are noted during the 1995–2009 period despite an increase in total vehicle distance traveled. The CO and NO_x emission trends are correlated with statistically significant downward trends in ambient air concentrations of CO and NO_x in Atlanta ranging from 8.0% to 11.8% per year and from 5.8% to 8.7% per year, respectively, during similar time periods. Weather-adjusted summertime ozone concentrations in Atlanta exhibited a statistically significant declining trend of 2.3% per year during 2001–2009. Although this trend coexists with the declining trends in on-road NO_x, VOC, and CO emissions, identifying the cause of the downward trend in ozone is complicated by reductions in multiple precursors from different source sectors.

Implications:Large reductions in on-road vehicle emissions of CO and NO_x in Atlanta from the late 1990s to 2009, despite an increase in total vehicle distance traveled, contributed to a significant improvement in air quality through decreases in ambient air concentrations of CO and NO_x during this time period. Emissions reductions in motor vehicles and other source sectors resulted in these improvements and the observed declining trend in ozone concentrations over the past decade. Although these historical trends cannot be extrapolated to the future because pollutant concentration contributions due to on-road vehicle emissions will likely become an increasingly smaller fraction of the atmospheric total, they provide an indication of the benefits of past control measures.     

Particulate matter in California: part 1--Intercomparison of several PM2.5, PM10-2.5, and PM10 monitoring networks

It will be many years before the recently deployed network of fine particulate matter with an aerodynamic diameter less than 2.5 microm (PM2.5) Federal Reference Method (FRM) samplers produces information on nonattainment areas, trends, and source impacts. However, data on PM2.5 and its major constituents have been routinely collected in California for the past 20 years. The California Air Resources Board operated as many as 20 dichotomous (dichot) samplers for PM2.5 and coarse PM (PM10-2.5). The California Acid Deposition Monitoring Program (CADMP) collected 12-h-average PM2.5 and PM10 from 1988 to 1995 at ten urban and rural sites and 24-h-average PM2.5 at five urban sites since 1995. Beginning in 1994, the Children's Health Study collected 2-week averages of PM2.5 in 12 communities in southern California using the Two-Week Sampler (TWS). Comparisons of collocated samples establish relationships between the dichot, CADMP, and TWS samplers and the 82-site network of PM2.5 FRM samplers deployed since 1999 in California. PM mass data from the different monitoring programs have modest to high correlation to FRM mass data, fairly small systematic biases and negative proportional biases ranging from 7 to 22%. If the biases are taken into account, all of the programs should be considered comparable with the FRM program. Thus, historical data can be used to develop long-term PM trends in California.     

Trends and Relationships of O3, NOx and HC in the South Coast Air Basin of California

A basin-wide air quality trend analysis for the South Coast Air Basin of California is conducted for hydrocarbons (HC), NO_x, O₃ and CO using multi-station composite daily maximum-hour average ambient concentrations for the third quarter (July, August and September) from 1968 to 1985. Emissions and air quality trends are compared for the period 1968-1984. Ambient HC and NOX trends are somewhat different from estimated emission trends of HC and NO_x, while a definite, downward trend of ambient CO is consistent with vehicular emission control measures. Basin-wide ambient HC, NO_x and O₃ appear to show downward trends for the period 1970-1985, but because of high fluctuations it is difficult to delineate trends for shorter periods. The meteorology (850 mb temperature)-adjusted O₃ shows a more consistent downward trend than does unadjusted O₃. Polynomial and multiplicative regression models for basin-wide empirical O₃-HC-NO_x relationships Indicate that the O₃ variation is explained largely by the meteorological variable (850 mb temperature) although model estimations are improved by adding HC and NO_x concentration terms.     

Remote Sensing Data and a Potential Model of Vehicle Exhaust Emissions

In June 1991, General Motors Research and Development Center (GMR&D) participated in a remote sensing study conducted by the California Air Resources Board and the U. S. Environmental Protection Agency. During this study, the GMR&D remote sensor was used to measure the carbon monoxide (CO) and hydrocarbon (HC) emissions from approximately 15,000 vehicles. The vehicle type (passenger car, light-duty truck, or medium/heavy-duty truck), manufacturer, and model year were identified for each vehicle by acquiring registration data from the state of California. Analyses were performed separately for each vehicle type and for passenger cars by separate model years. The data indicate that the passenger cars with the highest 10% of CO emissions generated approximately 58% of the total CO from all cars. Similarly, the 10% highest HC-emitting cars generated 65% of the total HC from cars. It was found that for each model year of vehicle, the distribution of emission concentrations followed a logarithmic relationship. The logarithmic functions that describe these relationships can be used to estimate the fraction of vehicles that emitted at or above any given concentration of CO or HC. However, these logarithmic functions only describe measured distributions for vehicles emitting more than 1% CO and 0.015% HC.     

Methodological trends in the design of recent microenvironmental studies of personal CO exposure

This paper describes the designs of three recent microenvironmental studies of personal exposure to carbon monoxide (CO) from motor vehicle exhaust. These studies were conducted sequentially, first in four California cities (Los Angeles, Mountain View, Palo Alto, and San Francisco), then in Honolulu, and, most recently, in metropolitan Washington, D.C. Though study purposes differed, each study faced common methodological issues related to personal exposure monitors (PEMs), quality assurance and data collection procedures, and the selection of microenvironments for study.Two major objectives of the California cities study were to determine the CO concentrations typically found in commercial settings and to define and classify microenvironments applicable to such settings: The Honolulu study measured merchant exposure to CO in shopping centers attached to semienclosed parking garages during business hours and commuter exposure to CO in vehicles (passenger cars and buses) on congested roadways during peak periods. The intent of the Washington study was to develop a model of commuter exposure to motor vehicle exhaust using CO as an indicator pollutant.Certain trends are discernible from reviewing the three studies. There are clearly trends in PEM development that have expanded instrument capabilities and automated data collection and storage. There are also trends towards more rigorous quality assurance procedures and more standardized protocols for collecting exposure data. Further, one can see a trend towards more elaborate indicators for identifying microenvironments for study. Finally, there is a trend towards using personal monitors in public policy review and evaluation.     

Trends in fine particle concentration and chemical composition in southern California

Airborne fine particle mass concentrations in Southern California have declined in recent years. Trends in sulfate and elemental carbon (EC) particle concentrations over the period 1982-1993 are consistent with this overall improvement in air quality and help to confirm some of the reasons for the changes that are seen. Fine particle sulfate concentrations have declined as a strict sulfur oxides (SOx) emission control program adopted in 1978 was implemented over time. Fine particle elemental (black) carbon concentrations have declined over a period when newer diesel engines and improved diesel fuels have been introduced into the vehicle fleet. Organic aerosol concentrations have not declined as rapidly as the EC particle concentrations, despite the fact that catalyst-equipped cars having lower particle emission rates were introduced into the vehicle fleet alongside the diesel engine improvements mentioned above. This situation is consistent with the growth in population and vehicle miles traveled in the air basin over time. Fine particle ammonium nitrate in the Los Angeles area atmosphere contributes more than half of the fine aerosol mass concentration on the highest concentration days of the year, emphasizing both the need for accurate aerosol nitrate measurements and the likely importance of deliberate control of aerosol nitrate as a part of any serious further fine particle control program for the Los Angeles area.     

Hot emission model for mobile sources: application to the metropolitan region of the city of Santiago, Chile

Depending on the final application, several methodologies for traffic emission estimation have been developed. Emission estimation based on total miles traveled or other average factors is a sufficient approach only for extended areas such as national or worldwide areas. For road emission control and strategies design, microscale analysis based on real-world emission estimations is often required. This involves actual driving behavior and emission factors of the local vehicle fleet under study. This paper reports on a microscale model for hot road emissions and its application to the metropolitan region of the city of Santiago, Chile. The methodology considers the street-by-street hot emission estimation with its temporal and spatial distribution. The input data come from experimental emission factors based on local driving patterns and traffic surveys of traffic flows for different vehicle categories. The methodology developed is able to estimate hourly hot road CO, total unburned hydrocarbons (THCs), particulate matter (PM), and NO(x) emissions for predefined day types and vehicle categories.     

Trends of PCDD/F and PCB concentrations and depositions in ambient air in Northwestern Germany

Time series of polychlorinated dioxins and furans (PCDD/F) and polychlorinated biphenyls (PCB) in ambient air of a large conurbation in North-Western Germany are presented and analyzed. The trend of PCDD/F concentrations, starting from as early as 1988, shows a pronounced decrease by at least one order of magnitude, demonstrating that the emission reductions were effective. The PCDD/F depositions also have decreased by a factor of 5 since 1992. However, both trends have leveled out since 2005. Time series of PCB concentrations and depositions starting in 1994 show only slight decreases for the concentrations and almost no decrease for the depositions. From the decay rates following first order kinetics, half-lives in the order of 5-15 years for the PCDD/F and 15-31 years for the sum of the six indicator PCB could be calculated, which are much longer than the half-lives estimated from their reactivity towards the OH radical. Apparently, small fresh emissions (PCDD/F), considerable secondary emissions and evaporation from contaminated soils slow down their decay in the atmosphere of big conurbations. Analyzing the decay rates of individual PCB congeners shows that the lower chlorinated and more volatile ones are removed faster than the higher chlorinated congeners, probably via gas phase reactions with the OH radical. It can be concluded from the present study that the input of PCDD/F and PCB into the food chain via the air path will continue for another one or two decades in big conurbations.     

A Mathematical Model for Predicting Trends in Carbon Monoxide Emissions and Exposures on Urban Arterial Highways

Abstract

The roadway is one of the most important microenvironments for human exposure to carbon monoxide (CO). To evaluate long-term changes in pollutant exposure due to in-transit activities, a mathematical model has been developed to predict average daily vehicular emissions on highways. By utilizing measurements that are specific for a given location and year (e.g., traffic counts, fleet composition), this model can predict emissions for a specific roadway during various time periods of interest, allowing examination of long-term trends in human exposure to CO. For an arterial highway in northern California, this model predicts that CO emissions should have declined by 58% between 1980 and 1991, which agrees fairly well with field measurements of human exposure taken along that roadway during those two years. An additional reduction of up to 60% in CO emissions is predicted to occur between 1991 and 2002, due solely to the continued replacement of older cars with newer, cleaner vehicles.     

Trends in passenger exposure to carbon monoxide inside a vehicle on an arterial highway of the San Francisco Peninsula over 30 years: A longitudinal study

This paper describes a long-term trend study of passenger exposure to carbon monoxide (CO) inside a vehicle traveling on an arterial highway in northern California. CO exposure was measured during four field surveys on State Route #82 (El Camino Real) on the San Francisco Peninsula in 1980–1981, 1991–1992, 2001–2002, and 2010–2011. Each field survey took at least 12 months. Fifty trips from each survey—for a total of 200 trips—were matched by date, day of the week, and starting time of the day to facilitate comparisons over three decades. The mean net CO concentration of each trip was obtained by subtracting the background CO level from the average CO concentration for the entire trip. The mean net CO concentration (0.5 ppm) for 2010–2011 was only 5.2% of that (9.7 ppm) for 1980–1981. For the 50 trips, the average travel time for the 1980–1981 period (39.6 min) was only 8.3% higher than during the 2010–2011 period (36.3 min). The estimated round-trip distance on the highway was held constant at 11.8 miles. The reduction in the mean net CO concentration was attributed to more stringent CO emission standards on new vehicles sold in California since 1980. The state’s cold-temperature CO standard implemented in 1996 appeared to reduce high CO concentrations that were observed during the late fall and winter of 1980–1981. In addition, the observed standard deviation in concentration fell from 3.1 ppm in 1980–1981 to 0.2 ppm in 2010–2011, and the range of the 50 mean net CO concentrations narrowed from 14.9 ppm in 1980–1981 to 1.1 ppm in 2010–2011, but the relative variability, as indicated by the geometric standard deviation, remained the same. These results have important scientific implications for regulatory policies designed to control air pollution from motor vehicles.

Implications: Many developing countries launched or expanded their mobile source emission control programs in the 1990s, yet many of them do not have adequate inspection and maintenance (I/M) programs. The El Camino Real study shows the long-term public health benefits of more stringent motor vehicle emission standards for carbon monoxide (CO) on new cars and of an I/M program (Smog Check) on the existing fleet in California. The study provides a protocol for conducting standardized field surveys of in-vehicle exposure on a periodic basis. Such surveys would enable developing countries to assess the progress of their mobile source emission control programs.     

NMOC,ozone, and organic aerosol in the southeastern United States, 1999–2007: 1. Spatial and temporal variations of NMOC concentrations and composition in Atlanta,Georgia

Volatile organic compounds (VOCs) are emitted from anthropogenic and natural (biogenic) sources into the atmosphere. Characterizing their ambient mixing ratios or concentrations is a challenge because VOCs comprise hundreds of species, and accurate measurements are difficult. Long-term hourly and daily-resolution data have been collected in the metropolitan area of Atlanta, Georgia, a major city dominated by motor vehicle emissions. A series of observations of daily, speciated C₂–C₁₀ non-methane organic compounds (NMOC) and oxygenated hydrocarbons (OVOC) in mid-town Atlanta (Jefferson Street, JST) are compared with data from three urban-suburban sites and a nearby non-urban site. Annual-average mixing ratios of NMOC and OVOC at JST declined from 1999 through 2007. Downward trends in NMOC, CO, and NO_y corroborate expected emission changes as reflected in emission inventories for Atlanta’s Fulton County. Comparison of the JST NMOC composition with data from roadside and tunnel sampling reveals similarities to motor vehicle dominated samples. The JST annual average VOC-OH reactivities from 1999 to 2007 were relatively constant compared with the decline in annual-average NMOC mixing ratios. Mean reactivity at JST, in terms of concentration*k_OH, was approximately 40% alkenes, 22% aromatics, 16% isoprene and 6% other biogenics, 13% C₇–C₁₀ alkanes and 3% C₂-C₆ alkanes, indicating that biogenic NMOCs are important but not dominant contributors to the urban reactive NMOC mix. In contrast, isoprene constituted ～50% of the VOC-OH reactivities at two non-urban sites. Ratios of 24-hour average CO/benzene, CO/isopentane, and CO/acetylene concentrations indicate that such species are relatively conserved, consistent with their low reactivity. Ratios of more-reactive to less-reactive species show diurnal variability largely consistent with expected emission patterns, transport and mixing of air, and chemical processing.     

Sensitivity Analysis and Evaluation of MicroFacCO: A Microscale Motor Vehicle Emission Factor Model for CO Emissions

ABSTRACT

This paper presents a sensitivity analysis of a microscale emission factor model (MicroFacCO) for predicting realtime site-specific motor vehicle CO emissions to input variables, as well as a limited field study evaluation of the model. The sensitivity analysis has shown that MicroFacCO emission estimates are very sensitive to vehicle fleet composition, speed, and ambient temperature. For the present U.S. traffic fleet, the CO emission rate (g/mi) is increased by more than 500% at 5 mph in comparison with a speed greater than 40 mph and by ~67% at ambient temperatures of 45 °F and ≥95 °F in comparison with an ambient temperature of 75 °F.     

Carbon Monoxide Exposures to Los Angeles Area Commuters

Carbon monoxide exposures to commuters were simulated in a 5-day study in Los Angeles County. Exposures were determined by measuring CO in three vehicles as they traveled typical commuter routes. The data collected during this study include measurements of vehicle speed and CO measurements in the interior and exterior of the three vehicles during the morning and evening peak traffic periods. In addition, hourly averaged CO measurements were taken from eight south coastal Air Quality Management District fixed-site monitoring stations and six California Department of Transportation vans in the proximity of the commuter routes. These data were used to investigate the relationship of CO exposures to meteorological parameters, fixed-site monitors, and traffic conditions.

The average ratio of interior CO concentrations to exterior CO concentrations was 0.92. Concentrations inside and outside the vehicles remained about the same even when the vehicles were driven with vents closed and windows up. Smoking was not permitted in the vehicles during the study. The average ratio of the hour average CO concentrations in the vehicles to fixed-site measurements was 3.9. However, this ratio decreases with increasing ambient CO levels. Although CO levels in the vehicles frequently exceeded 40 ppm and sometimes exceeded 60 ppm, the hour average CO concentrations did not exceed 35 ppm. Slow moving congested traffic is associated with higher CO levels in the vehicles than a high volume of traffic moving at a steady speed.     

Changes of emissions and atmospheric deposition of mercury,lead, and cadmium

This paper reviews the information on trends of past emissions of mercury, lead, and cadmium in Europe, as well as examines current levels and future scenarios of these emissions. The impact of various factors on emission changes is discussed including the implementation of various strategies of emission controls in Europe. Future emissions are forecasted on the basis of various scenarios of economy growth in Europe, implementation of European and global legislation (e.g. the Kyoto agreement), population changes, etc.Changes of emissions of mercury, lead, and cadmium are then related to the changes of concentrations of these contaminants in air and precipitation samples at selected stations in Europe. It can be concluded that the reduction trends of anthropogenic emissions of cadmium and lead in Europe are similar to the reduction trends of air concentrations of these metals during the last 2 decades. Somewhat different relationship has been noted for changes in emissions and precipitation. In general for Europe, 60% reduction of Cd emissions was met by about 45% reductions of Cd concentrations in precipitation at the studied stations during the last 2 decades.There is a potential for further reduction of these emissions until the year 2010 up to about 37% for Cd, 51% for Pb, and 49% for Hg as estimated within various emission scenarios presented in the paper.     

Measured carbon monoxide concentrations from stock and reduced-emission prototype portable generators operated in an attached garage

There is concern about the hazard of acute residential CO exposures from portable gasoline-powered generators, which can result in death or serious adverse health effects in exposed individuals. To address this hazard, the U.S. Consumer Product Safety Commission has developed low CO emission prototype generators by adapting off-the-shelf emission control technologies onto commercially available generators. A series of tests was conducted to characterize the indoor CO concentrations resulting from portable generators operating in the attached garage of a research house under seven different test house/garage configurations. The tested generators include both unmodified and modified low CO emission prototypes. It was found that CO concentrations varied widely, with peak house CO concentrations ranging from under 10 ppm to over 10,000 ppm. The highest concentrations in the house resulted from operation of the unmodified generator in the garage with the garage bay door closed and the house access door open. The lowest concentrations resulted from operation of a modified low CO emission prototype in the garage with the garage bay door open and the house access door closed. These tests documented reductions of up to 98% in CO concentrations due to emissions from two low CO emission portable generators compared to a stock generator.

Implications: Improper portable generator use has caused 800 U.S. deaths in the past 14 years. Generators operated in attached garages can cause CO to quickly reach deadly levels. Two low-emission prototypes generators were tested and had CO emissions reduced by up to 98%. Low-emission generators can reduce the risk of consumer poisonings and deaths.     

Ammonia emissions from a representative in-use fleet of light and medium-duty vehicles in the California South Coast Air Basin

We used Fourier Transform Infrared Spectroscopy (FTIR) to measure tailpipe ammonia emissions from a representative fleet of 41 light and medium-duty vehicles recruited in the California South Coast Air Basin. A total of 121 chassis dynamometer emissions tests were conducted on these vehicles and the test results were examined to determine the effects of several key variables on ammonia emissions. Variables included vehicle type, driving cycle, emissions technology, ammonia precursor emissions (i.e. CO and NOx) and odometer readings/model year as a proxy for catalyst age. The mean ammonia emissions factor was 46 mg km^?1 (σ = 48 mg km^?1) for the vehicle fleet. Average emission factors for specific vehicle groups are also reported in this study. Results of this study suggest vehicles with the highest ammonia emission rates possess the following characteristics: medium-duty vehicles, older emissions technologies, mid-range odometer readings, and higher CO emissions. In addition, vehicles subjected to aggressive driving conditions are likely to be higher ammonia emitters. Since the vehicles we studied were representative of recent model year vehicles and technologies in urban airsheds, the results of our study will be useful for developing ammonia emissions inventories in Los Angeles and other urban areas where California-certified vehicles are driven. However, efforts should also be made to continue emissions testing on in-use vehicles to ensure greater confidence in the ammonia emission factors reported here.     

Trends in vehicular emissions in China's mega cities from 1995 to 2005

Multiyear inventories of vehicular emissions in Beijing, Shanghai and Guangzhou from 1995 through 2005 have been developed in this paper to study the vehicle emissions trends in China's mega cities during the past decade. The results show that the vehicular emissions of CO, HC, NO_x and PM₁₀ have begun to slow their growth rates and perhaps even to decline in recent years due to the implementation of measures to control vehicular emissions in these cities. However, vehicular CO₂ emissions have substantially increased and still continue to grow due to little fuel economy improvement. Passenger cars and large vehicles (including heavy duty trucks and buses) are the major sources of vehicular CO₂ and CO emissions while large vehicles were responsible for nearly 70% and 80% of the vehicular NO_x and PM₁₀ emissions in these mega cities. Motorcycles are also important contributors to vehicular emissions in Guangzhou and Shanghai.     

Development of a microscale emission factor model for particulate matter for predicting real-time motor vehicle emissions

The U.S. Environmental Protection Agency's National Exposure Research Laboratory is pursuing a project to improve the methodology for modeling human exposure to motor vehicle emissions. The overall project goal is to develop improved methods for modeling the source through the air pathway to human exposure in significant exposure microenvironments. Current particulate matter (PM) emission models, particle emission factor model (used in the United States, except California) and motor vehicle emission factor model (used in California only), are suitable only for county-scale modeling and emission inventories. There is a need to develop a site-specific real-time emission factor model for PM emissions to support human exposure studies near roadways. A microscale emission factor model for predicting site-specific real-time motor vehicle PM (MicroFacPM) emissions for total suspended PM, PM less than 10 microm aerodynamic diameter, and PM less than 2.5 microm aerodynamic diameter has been developed. The algorithm used to calculate emission factors in MicroFacPM is disaggregated, and emission factors are calculated from a real-time fleet, rather than from a fleet-wide average estimated by a vehicle-miles-traveled weighting of the emission factors for different vehicle classes. MicroFacPM requires input information necessary to characterize the site-specific real-time fleet being modeled. Other variables required include average vehicle speed, time and day of the year, ambient temperature, and relative humidity.