Evolution of particulate regulation in China--prospects and challenges of exposure-based control

China's urban and rural populations face very serious health risks from combustion particles. Major sources of exposure to inhalable particulates include the burning solid fuels (biomass and coal) for household cooking and heating, coal-fired industrial and residential boilers, tobacco smoking, and diesel motor vehicles. China began to address particulate pollution problems over 25 years ago and has implemented a series of progressively more aggressive policies. This paper reviews the successes and limitations of past and existing policies for particulate controls, as well as the effects of China's economic reforms and energy policies on particulate exposure and pollution management. We examine the challenge of emissions reporting, required as part of both China's pollution levy system and emerging system for "total emissions control." Finally, we discuss practical steps toward exposure-based regulation of particulates, which would take advantage of the high cost-effectiveness for lifesaving of controlling particulate exposure from household and neighborhood sources relative to that of controlling exposure from industrial sources.     

Daily Variability of Motor Vehicle Emissions Derived from Traffic Counter Data

ABSTRACT

This work studied the daily variability of mobile sources in rural and urban areas, in and around the Atlanta Metropolitan Area. Traffic counter data collected during the 1992 Southern Oxidants Study Atlanta Intensive Study were used to analyze the spatial and temporal distribution of traffic volume. A simple method to study the daily variability of mobile emissions from the different types of urban and rural roads is presented. The method is based on hourly traffic volume data and emission factors and it has been generalized to describe the daily variability of mobile emissions for urban and rural areas and for the whole modeling domain. Implications of this study for improving mobile emission inventories are also discussed.     

Different sources of rural household energy consumption and influencing factors in Dazu,China

Rural household energy consumption is an important component of national energy consumption. This paper explores the rural household energy consumption status and influencing factors on different sources of rural household energy consumption in western China. Using data from a survey of 240 households conducted in 2017, this study finds that rural households’ energy consumption structure in the study area is a combination of traditional biomass energy and commercial energy sources. Fuelwood is the most commonly used fuel in the study area, while modern energy sources only occupy a low proportion. Rural household energy consumption is influenced by various factors. Individual perceptions of climate change, social trust and networks, and households’ socio-economic and demographic factors (gender, age, education, income per capita, household size, household location, and number of household appliances) are identified as having significant effects on rural households’ consumption of biomass and commercial energies. The research results provide implications for policy makers to formulate related rural energy policies to improve the rural energy consumption structure and future energy policy design in China and other developing countries.

     

C1–C8 volatile organic compounds in the atmosphere of Hong Kong: Overview of atmospheric processing and source apportionment

We present measurements of C₁–C₈ volatile organic compounds (VOCs) at four sites ranging from urban to rural areas in Hong Kong from September 2002 to August 2003. A total of 248 ambient VOC samples were collected. As expected, the urban and sub-urban sites generally gave relatively high VOC levels. In contrast, the average VOC levels were the lowest in the rural area. In general, higher mixing ratios were observed during winter/spring and lower levels during summer/fall because of seasonal variations of meteorological conditions. A variation of the air mass composition from urban to rural sites was observed. High ratios of ethyne/CO (5.6 pptv/ppbv) and propane/ethane (0.50 pptv/pptv) at the rural site suggested that the air masses over the territory were relatively fresh as compared to other remote regions. The principal component analysis (PCA) with absolute principal component scores (APCS) technique was applied to the VOC data in order to identify and quantify pollution sources at different sites. These results indicated that vehicular emissions made a significant contribution to ambient non-methane VOCs (NMVOCs) levels in urban areas (65±36%) and in sub-urban areas (50±28% and 53±41%). Other sources such as petrol evaporation, industrial emissions and solvent usage also played important roles in the VOC emissions. At the rural site, almost half of the measured total NMVOCs were due to combustion sources (vehicular and/or biomass/biofuel burning). Petrol evaporation, solvent usage, industrial and biogenic emissions also contributed to the atmospheric NMVOCs. The source apportionment results revealed a strong impact of anthropogenic VOCs to the atmosphere of Hong Kong in both urban/sub-urban and rural areas.     

Nonmethane Organic Compound to Nitrogen Oxide Ratios and Organic Composition in Cities and Rural Areas

The observed ranges in nonmethane organic compound (NMOC) concentrations, NMOC composition and nitrogen oxides (NO_X) concentrations have been evaluated for urban and nonurban areas at ground level and aloft of the contiguous United States. The ranges in NMOC to NO_X ratios also are considered. The NMOC composition consistently shifts towards less reactive compounds, especially the alkanes, in air parcels over nonurban areas compared to the NMOC composition near ground level within urban areas. The values for the NMOC to NO_X ratios, 1.2 to 4.2, in air aloft over nonurban areas are lower than in air at ground level urban sites, ≥8, and much lower than in air at ground level nonurban sites, ≥20.

The layers of air aloft over a number of nonurban areas of the United States tend to accumulate NO_X emissions from the tall stacks of large fossil fuel power plants located at nonurban sites. During the night into the morning hours, the air aloft is isolated from any fresh NMOC emissions predominately coming from near surface sources. Conversely, during this extended period of restricted vertical mixing, air near the surface accumulates NMOC emissions while this air is isolated from the major NO_X sources emitting aloft. These differences in the distribution of NMOC and NO_X sources appear to account for the much larger NMOC to NO_X ratios reported near ground level compared to aloft over nonurban areas.

Two types of experimental results are consistent with these conclusions: (1) observed increases in surface rural NO_X concentrations during the morning hours during which the mixing depth increases to reach the altitude at which NO_X from the stacks of fossil fuel power plants is being transported downwind; (2) high correlations of total nitrate at rural locations with Se, which is a tracer for coal-fired power plant NO_X emissions.

The implications of these conclusions from the standpoint of air quality strategies are suggested by use of appropriate scenarios applied to both urban and regional scale photochemical air quality models. The predictions from urban model scenarios with NMOC to NO_X ratios up to 20 are that NO_X control will result in the need for the control of more NMOC emissions than necessary in the absence of NO_X control, in order to meet the O₃ standard. On a regional scale, control of NO_X emissions from fossil fuel power plants has little overall effect regionally but does result on a more local scale in both small decreases and increases in O₃ concentrations compared to the baseline scenario without NO_X control. The regional modeling results obtained to date suggest that NO_X control may be effective in reducing O₃ concentrations only for a very limited set of conditions in rural areas.     

Effects of biodiesel made from swine and chicken fat residues on carbon monoxide,carbon dioxide,and nitrogen oxide emissions

The effects of two alternative sources of animal fat-derived biodiesel feedstock on CO₂, CO, NO_x tailpipe emissions as well as fuel consumption were investigated. Biodiesel blends were produced from chicken and swine fat waste (FW-1) or floating fat (FW-2) collected from slaughterhouse wastewater treatment processes. Tests were conducted in an unmodified stationary diesel engine operating under idling conditions in attempt to simulate slow traffic in urban areas. Significant reductions in CO (up to 47% for B100; FW-2) and NO_x (up to 20% for B5; FW-2 or B100; FW-1) were attained when using biodiesel fuels at the expense of 5% increase in fuel consumption. Principal component analysis (PCA) was performed to elucidate possible associations among gas (CO₂, CO, and NO_x) emissions, cetane number and iodine index with different sources of feedstock typically employed in the biodiesel industry. NO_x, cetane number and iodine index were inversely proportional to CO₂ and biodiesel concentration. High NO_x emissions were reported from high iodine index biodiesel derived especially from forestry, fishery and some agriculture feedstocks, while the biodiesel derived from animal sources consistently presented lower iodine index mitigating NO_x emissions. The obtained results point out the applicability of biodiesel fuels derived from fat-rich residues originated from animal production on mitigation of greenhouse gas emissions. The information may encourage practitioners from biodiesel industry whilst contributing towards development of sustainable animal production.

Implications: Emissions from motor vehicles can contribute considerably to the levels of greenhouse gases in the atmosphere. The use of biodiesel to replace or augment diesel can not only decrease our dependency on fossil fuels but also help decrease air pollution. Thus, different sources of feedstocks are constantly being explored for affordable biodiesel production. However, the amount of carbon monoxide (CO), carbon dioxide (CO₂), and/or nitrogen oxide (NO_x) emissions can vary largely depending on type of feedstock used to produce biodiesel. In this work, the authors demonstrated animal fat feasibility in replacing petrodiesel with less impact regarding greenhouse gas emissions than other sources.     

Concentrations, sources and spatial distribution of polycyclic aromatic hydrocarbons in soils from Beijing, Tianjin and surrounding areas, North China

The concentrations, profiles, sources and spatial distribution of polycyclic aromatic hydrocarbons (PAHs) were determined in 40 surface soil samples collected from Beijing, Tianjin and surrounding areas, North China in 2007, and all sampling sites were far from industrial areas, roadsides and other pollution sources, and across a range of soil types in remote, rural villages and urban areas. The total concentrations of 16 PAHs ranged from 31.6 to 1475.0 ng/g, with an arithmetic average of 336.4 ng/g. The highest PAH concentrations were measured in urban soils, followed by rural village soils and soils from remote locations. The remote-rural village-urban PAH concentration gradient was related to population density, gross domestic product (GDP), long-range atmospheric transport and different types of land use. In addition, the PAH concentration was well correlated with the total organic carbon (TOC) concentration of the soil. The PAH profile suggested that coal combustion and biomass burning were primary PAH sources.     

Toxic Emissions from Mobile Sources: A Total Fuel-Cycle Analysis for Conventional and Alternative Fuel Vehicles

ABSTRACT

Mobile sources are among the largest contributors of four hazardous air pollutants—benzene, 1,3-butadiene, acetal-dehyde, and formaldehyde—in urban areas. At the same time, federal and state governments are promoting the use of alternative fuel vehicles as a means to curb local air pollution. As yet, the impact of this movement toward alternative fuels with respect to toxic emissions has not been well studied. The purpose of this paper is to compare toxic emissions from vehicles operating on a variety of fuels, including reformulated gasoline (RFG), natural gas, ethanol, methanol, liquid petroleum gas (LPG), and electricity. This study uses a version of Argonne National Laboratory's Greenhouse Gas, Regulated Emissions, and Energy Use in Transportation (GREET) model, appropriately modified to estimate toxic emissions. The GREET model conducts a total fuel-cycle analysis that calculates emissions from both downstream (e.g., operation of the vehicle) and upstream (e.g., fuel production and distribution) stages of the fuel cycle. We find that almost all of the fuels studied reduce 1,3-buta-diene emissions compared with conventional gasoline (CG). However, the use of ethanol in E85 (fuel made with 85% ethanol) or RFG leads to increased acetaldehyde emissions, and the use of methanol, ethanol, and compressed natural gas (CNG) may result in increased formaldehyde emissions. When the modeling results for the four air toxics are considered together with their cancer risk factors, all the fuels and vehicle technologies show air toxic emission reduction benefits.     

Carbonaceous species in fine particles at the background sites in Korea between 1994 and 1999

Organic carbon (OC) and elemental carbon (EC) in fine particles (PM_2.5) at two background sites, Kosan and Kangwha in Korea were measured during intensive field studies between 1994 and 1999. Fine particles were collected on pre-fired quartz filters in a low-volume sampler and analyzed using the selective thermal oxidation method with MnO₂ catalyst. The OC and EC concentrations at Kosan located at western tip of Cheju Island in southern Korea are lower than those at Kangwha located at western coastal area in mid-Korean peninsula. Still, the OC concentrations at Kosan are generally higher than those at other background areas in Japan and USA. The EC concentrations at Kosan are lower than or comparable to those at other background areas. The total carbon (TC, sum of OC and EC) to EC ratio values at both sites were higher than those at other background areas in Japan and USA. At Kosan, the OC and EC concentrations when air parcels were from southern China were higher than those when air parcels were coming from northern China. However, at Kangwha, the differences were statistically not clear since most air parcels were from northern China. Except when air parcels were from the North Pacific during summer, the OC and EC concentrations are well correlated indicating that both OC and EC share the same emission/transport characteristics. From the gaseous hydrocarbon data and the OC and EC relationship, it was found that during summer local biogenic emissions of OC might be significant at Kosan.     

Seasonal Impact of Blending Oxygenated Organics with Gasoline on Motor Vehicle Tailpipe and Evaporative Emissions

Emissions from a 1988 GM Corsica with adaptive learning closed loop control were measured with 4 fuels at 40, 75, and 90° F. Evaporative and exhaust emissions were examined from each fuel at each test temperature. Test fuels were unleaded summer grade gasoline; a blend of this gasoline containing 8.1 percent ethanol; a refiner’s blend stock; and the blend stock containing 16.2 percent methyl tertiary butyl ether. The ethanol and MTBE blends contained 3.0 percent oxygen by weight. Regulated emissions (total hydrocarbons, carbon monoxide, and oxides of nitrogen), detailed aldehydes, detailed hydrocarbons, ethanol, MTBE, benzene, and 1, 3-butadiene were determined.

The highest levels of regulated emissions were produced at the lower temperature. Blended fuels produced almost twice the evaporative hydrocarbon emissions at high temperatures as did the base fuels. Benzene emissions varied with fuels and operating temperatures, while 1, 3-butadiene emissions decreased slightly with increasing temperatures. Formaldehyde emissions were not sensitive to fuel or temperature changes. Ethanol fuel blend total aldehyde emissions Increased by 40 percent due to increased acetaldehyde emissions.

Fuel blends had approximately a 3 percent economy decrease. The MTBE fuel blend appeared to offer the most reduction in total hydrocarbon, carbon monoxide, and oxides of nitrogen for the fuels and temperatures tested.     

我国氮氧化物排放因子的修正和排放量计算:2000年

根据我国城市的发展状况 ,采用城市分类的方法 ,将我国 2 6 1个地级市按照人口数量分为 5个类别。每类城市选取一个典型城市进行实地调查 ,对我国燃烧锅炉和机动车的NOx 的排放因子进行了修正 ,提出了适合我国目前排放水平的各类城市的固定源和移动源的排放因子。并依据 2 0 0 0年中国大陆地区的电站锅炉、工业锅炉和民用炉具的燃料消耗量和机动车保有量 ,以地级市为基本单位 ,估算了 2 0 0 0年我国各地区的NOx 排放量 ,分析了分地区、分行业、分燃料类型的NOx 排放特征。 2 0 0 0年我国NOx 排放总量为 11.12Mt,其中固定源占 6 0 .8% ;移动源占 39.2 %。NOx 排放在地域、行业和燃料类型上分布均不平衡。NOx 的排放主要集中在华东和华北地区 ,其排放量占全国排放量的一半以上。燃煤为最重要的NOx 排放源 ,其排放量占燃料型NOx 排放量的 72 .3%左右。     

On the local and regional influence on ground-level ozone concentrations in Hong Kong

Hong Kong is a densely populated city situated in the fast developing Pearl River Delta of southern China. In this study, the recent data on ozone (O3) and related air pollutants obtained at three sites in Hong Kong are analyzed to show the variations of O3 in urban, sub-urban and rural areas and the possible regional influences. Highest monthly averaged O3 was found at a northeastern rural site and lowest O3 level was observed at an urban site. The levels of NOx, CO, SO2 and PM10 showed a different spatial pattern with the highest level in the urban site and lowest at the rural site. Analysis of chemical species ratios such as SO2/NOx and CO/NOx indicated that the sites were under the influences of local and regional emissions to varying extents reflecting the characteristics of emission sources surround the respective sites. Seasonal pattern of O3 is examined. Low O3 level was found in summer and elevated levels occurred in autumn and spring. The latter appears different from the previous result obtained in 1996 indicating a single maximum occurring in autumn. Principal component analysis was used to further elucidate the relationships of air pollutants at each site. As expected, the O3 variation in the northeastern rural area was largely determined by regional chemical and transport processes, while the O3 variability at the southwestern suburban and urban sites were more influenced by local emissions. Despite the large difference in O3 levels across the sites, total potential ozone (O3+NO2) showed little variability. Cases of high O3 episodes were presented and elevated O3 levels were formed under the influence of tropical cyclone bringing in conditions of intense sunlight, high temperature and light winds. Elevated O3 levels were also found to correlate with enhanced ratio of SO2 to NOx, suggesting influence of regional emissions from the adjacent Pearl River Delta region.     

A Comparison of Measured and Simulated Ozone Concentrations in the Rural Areas of the Eastern United States during Summer 1995

ABSTRACT

The recent regulatory actions toward a longer-term (i.e., 8-hr) average ozone standard have brought forth the potential for many rural areas in the eastern United States to be in noncompliance. However, since a majority of these rural areas have generally few sources of anthropogenic emissions, the measured ozone levels primarily reflect the effects of the transport of ozone and its precursor pollutants and natural emissions. While photochemical grid models have been applied to urban areas to develop ozone mitigation measures, these efforts have been limited to high ozone episode events only and do not adequately cover rural regions. In this study, we applied a photochemical modeling system, RAMS/UAM-V, to the eastern United States from June 1-August 31, 1995. The purpose of the study is to examine the predictive ability of the modeling system at rural monitoring stations that are part of the Clean Air Status Trends Network (CASTNet) and the Gaseous Pollutant Monitoring Program (GPMP).

The results show that the measured daily 1-hr ozone maxima and the seasonal average of the daily 1-hr ozone maxima are in better agreement with the predictions of the modeling system than those for the daily 8-hr ozone maxima. Also, the response of the modeling system in reproducing the measured range of ozone levels over the diurnal cycle is poor, suggesting the need for improvement in the treatment of the physical and chemical processes of the modeling system during the nighttime and morning hours if it is to be used to address the 8-hr ozone standard.     

Cheaper Fuel and Higher Health Costs Among the Poor in Rural Nepal

Biomass fuels are used by the majority of resource poor households in low-income countries. Though biomass fuels, such as dung-briquette and firewood are apparently cheaper than the modern fuels indoor pollution from burning biomass fuels incurs high health costs. But, the health costs of these conventional fuels, mostly being indirect, are poorly understood. To address this gap, this study develops probit regression models using survey data generated through interviews from households using either dung-briquette or biogas as the primary source of fuel for cooking. The study investigates factors affecting the use of dung-briquette, assesses its impact on human health, and estimates the associated household health costs. Analysis suggests significant effects of dung-briquette on asthma and eye diseases. Despite of the perception of it being a cheap fuel, the annual health cost per household due to burning dung-briquette (US16.94) is 61.3 (US 16.94) is 61.3% higher than the annual cost of biogas (US 10.38), an alternative cleaner fuel for rural households. For reducing the use of dung-briquette and its indirect health costs, the study recommends three interventions: (1) educate women and aboriginal people, in particular, and make them aware of the benefits of switching to biogas; (2) facilitate tree planting in communal as well as private lands; and (3) create rural employment and income generation opportunities.     

Receptor Modeling Applied to Patterns in Space (RMAPS)Part III–Apportionment of Airborne Particulate Sulfur in Western Washington State

Abstract

Data obtained from 24 of the 31 sites of the Pacific Northwest Regional Visibility Experiment Using Natural Tracers (PREVENT) study were analyzed by the Receptor Model Applied to Patterns in Space (RMAPS) multivariate receptor model. Four spatial patterns were found and interpreted as showing the effect of the coal-fired power plant in Centralia, WA; transport from the northwest; the Se-attle-Tacoma urban area; and transport from the southeast. In Mt. Rainier National Park, up to one-third of the sulfate can be attributed to the Centralia power plant. In the North Cascades National Park, 65-82% of the sulfur is accounted for by transport from Canada. The model was applied separately to sites in the northern and southern sections of the study area. The southern sites were affected only by the Centralia, urban, and southeast transport sources; the northern sites were affected only by the northwest transport, urban, and southeast transport sources. This gave two independent estimates of the normalized source contributions of the urban and southeast transport factors, which had a correlation coefficient of more than 0.90.     

Particulate air pollution from combustion and construction in coastal and urban areas of China

In China, the areas that are undergoing rapid urban growth are faced with increasingly more complicated air pollution problems. Sources of air pollution need to be identified and their contributions quantified. In this study, PM2.5 (particulate matter with aerodynamic diameters < or =2.5 microm), PM2.5-10 (particulate matter with aerodynamic diameters 2.5-10 microm), organic carbon (OC), and elemental carbon (EC) concentrations were measured from April to July 2009 at four selected areas in Xiamen (the downtown area, an industrial park, a suburb, and one remote site). The contributions of carbonaceous aerosols to PM2.5 and PM2.5-10 were 20-30% and 10-20%, respectively, indicating that finer particles contained more carbonaceous aerosols. The EC concentrations in PM2.5 at the downtown, industrial, suburb, and remote sites were 2.16 +/- 0.61, 2.05 +/- 0.45, 1.69 +/- 0.54, and 0.65 +/- 0.43 microg m-3, respectively, showing a decrease from the urban and industrial hotspots to the surrounding areas. These data show that carbonaceous aerosols emitted from the combustion of fossil fuels in urban and industrial hotspots influence air quality at the regional scale. Higher levels of PM2.5 and PM2.5-10 were observed at the suburb site compared to the urban and industrial sites. Peak EC concentrations in PM2.5 were observed during the morning and evening rush hours. However, peak PM2.5 levels at the suburb site were observed around noon, which coincides with construction work hours, instead of the morning and evening rush hours when emissions from combustion dominated. These findings indicate that both fuel combustion and construction have exacerbated air pollution in coastal and urban areas in China.     

Characteristics of organic matter in PM2.5 in Shanghai

Solvent extractable organic compounds (SEOC), organic carbon, elemental carbon and water soluble organic carbon (WSOC) in PM(2.5) samples collected in Shanghai, China in 2002 and 2003 were measured to determine the composition and sources of the organic matter in atmospheric aerosols. Distinct seasonal variations were detected with higher concentrations of organic matter in winter. The concentration of total carbon of about 20 microg m(-3) in winter was about three times the summer value. About 30% of the total carbon was water soluble. Unresolved complex mixture (UCM) and fatty acids were the most abundant components quantified in SEOC, similar to other Chinese cities previously studied. High ratio of UCM to n-alkanes (U:R) and the composition of triterpanes indicated that engine exhaust was a major source of the airborne organic matter. Emissions from coal burning had more impact in the rural areas, according to the U:R value and PAHs composition. Chemical mass balance (CMB) modeling shows that about half of the organic carbon was from engine exhaust and about 15% was from coal burning. No clear spatial variation in the concentration of the organic matter was found between urban and rural areas. Our results showed that due to the rapid urbanization and relocation of industrial plants from urban areas to rural areas in the past 20 years, air pollution in rural areas is becoming a serious problem in Shanghai and the Yangtze River delta.     

Control of Contaminant Emissions From Fossil Fuel-Fired Boilers

The importance of fuels combustion was brought into sharp focus recently in a report on air pollution to the United States Senate in which it was stated, “These processes replace usable air with potentially harmful pollutants, and the capability of the atmosphere to disperse and dilute these pollutants—especially in urban areas where people, vehicles, and industries congregate in even greater numbers—is strictly limited.”¹ The overwhelming burden of emissions of sulfur compounds, as well as nitrogen compounds and particulate matter in the U. S. today, originates from the burning of coal and fuel oil in stationary combustion sources. Thus, combustion has a large influence on the quality of the atmosphere in most urban areas. The air pollution effects of these contaminants are many and varied and all are objectionable and undesirable. Without a doubt, the most serious air pollution problem in the nation today is that created by the combustion of fossil fuels.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Spatial distribution of source locations for particulate nitrate and sulfate in the upper-midwestern United States

Two back-trajectory analysis methods designed to be used with multiple site data, simplified quantitative transport bias analysis (SQTBA) and residence time weighted concentration (RTWC), were applied to nitrate and sulfate concentration data from two rural sites (the Mammoth Cave National Park and the Great Smoky Mountain National Park) and five urban sites (Chicago, Cleveland, Detroit, Indianapolis, and St. Louis) for an intensive investigation on the spatial patterns of origins for these two species in the upper-midwestern area. The study was made by dividing the data into five categories: all sites and all seasons, rural sites in summer, rural sites in winter, urban sites in summer, and urban sites in winter. A general conclusion was that the origins of the nitrate in these seven sites were mainly in the upper-midwestern areas, while the sulfate in these seven sites were mainly from the Ohio and Tennessee River Valley areas. The upper-midwestern areas are regions of high ammonia emissions rather than high NO_x emissions. In the winter, metropolitan areas showed the highest nitrate emission potential suggesting the importance of local NO_x emissions. In the summer, ammonia emissions from fertilizer application in the lower midwestern area made a significant contribution to nitrate in the rural sites of this study. The impact of the wind direction prevalence on the source spatial patterns was observed by comparing the urban and rural patterns of the summer. The differences between the results of two methods are discussed and suggestions for applying these methods are also provided.