Spatial and temporal trends of precipitation chemistry in the United States, 1985-2002

A Seasonal Kendall Trend (SKT) test was applied to precipitation-weighted concentration data from 164 National Atmospheric Deposition Program National Trends Network (NADP/NTN) sites operational from 1985 to 2002. Analyses were performed on concentrations of ammonium, sulfate, nitrate, dissolved inorganic nitrogen (DIN, sum of nitrogen from nitrate and ammonium), and earth crustal cations (ECC, sum of calcium, magnesium, and potassium). Over the 18-year period, statistically significant (p< or =0.10) increases in ammonium concentrations occurred at 93 sites (58%), while just three sites had statistically significant ammonium decreases. Central and northern Midwestern states had the largest ammonium increases. The generally higher ammonium concentrations were accompanied by significant sulfate decreases (139 sites, 85%), and only one significant increase which occurred in Texas. In the west central United States there were significant nitrate increases (45 sites, 27%), while in the northeastern United States there were significant decreases (25 sites, 15%). Significant DIN decreases were observed in the northeastern United States (11 sites, 7%); elsewhere there were significant increases at 75 sites (46%). ECC decreased significantly at 65 sites (40%), predominantly in the central and southern United States, and increased at 11 sites (7%). The concentrations of sulfate, nitrate, and ammonium in precipitation have changed markedly over the time period studied. Such trends indicate changes in the mix of gases and particles scavenged by precipitation, possibly reflecting changes in emissions, atmospheric chemical transformations, and weather patterns.     

Spatial analysis of extreme precipitation in Sweden 1961-2000

Extreme daily precipitation in Sweden for the years 1961-2000 is analyzed with respect to spatial scale, regional variations and associated weather types. Correlograms based on a lag distance of 30 km estimated the spatial scale of variation of the annual mean precipitation, the 99th percentile of daily precipitation and the average of annual maximum daily precipitation to 100 km, 60-100 km and 40-70 km, respectively. Regions of correlation with respect to precipitation at 82 stations during days of extreme events are identified through Maximum-Likelihood Factor Analysis. Eleven factors are found to provide the optimum factor solution. Weather types for the days of extreme events are determined by an objective classification scheme, based on daily sea level pressure, which is modified by subjective inclusion of fronts. In total, 63% of the extreme events occurred during cyclonic weather types, 32% during frontal, 3% during directional and 2% during anticyclonic types. The frequency of the weather types during extreme events varied between the regions however.     

Phosphorus recovery from wastewater--expert survey on present use and future potential

Today, a variety of different approaches to the recovery of phosphorus from wastewater, sludge, and sludge ash exist. These approaches differ basically by the origin of the used matter (wastewater, sludge liquor, fermented or nonfermented sludge ash) and the process (precipitation, wet-chemical extraction, and thermal treatment). To rate them according to their characteristics, the latter were phrased as hypotheses and subjected to an international expert survey. The survey showed that phosphorus recovery is expected to become an established process over the next 20 years in industrialized countries for economic reasons. A decisive aspect in this regard will be the quality of the produced fertilizer. Simple technologies such as the recovery from sludge liquor seem to be preferred. If sludge is incinerated, phosphorus recycling from ash then becomes more interesting and has to be considered. Phosphorus recovery and source-separating sanitation technologies are more appropriate for industrialized countries than for developing countries. Because the growing awareness of environmental issues will prevent sludge from being used agriculturally in an increasing number of countries in the next decade, the market potential for nutrient recovery technologies will increase in the immediate future.     

Seasonal aerosol sulfate trends for selected regions of the United States

Site and regional trends in seasonally averaged particle SO4(2-) concentrations were examined for a large portion of the United States using data collected by the CASTNet air monitoring network. Trends were analyzed for overlapping periods of 1988-1999 and 1992-1999. The largest absolute SO4(2-) decreases--approximately -0.4 microg/m3/yr--between 1988 and 1999 occurred in summer for sites in the Ohio River Valley and areas to the east. Generally, the largest SO4(2-) reductions were found for summer, but larger relative reductions often occurred for spring and autumn. Sulfate changes during 1992-1999 were quite different from those found for 1988-1999 and were not entirely consistent with changes in SO2 emissions. In some locations, the 1992-1999 period saw smaller declines in SO4(2-), while in other places seasonal SO4(2-) actually increased. Increases were mostly confined to summer and autumn across the southern and southwestern states. Multivariate analysis of ambient sulfur levels, by region, versus SO2 emissions reveals that annual emissions are associated with more than 80% of the variance in seasonal sulfur (SO2 and SO4(2-)) in more than three-quarters of the cases examined. The weakest associations were found for the southeastern United States.     

Ammonia and ammonium measurements from the southeastern United States

Twenty-four-hour integrated gaseous ${\mathrm{NH}}_3$ and fine particulate $({\mathrm{PM}}_{2.5}){\mathrm{NH}}_4^{+}$ were measured during 2004 at eight sites in the southeastern U.S. Mean ${\mathrm{NH}}_3$ concentrations for 2004 ranged from 2.44 ppbv at an urban-industrial site in North Birmingham, AL, to 0.23 ppbv at a rural-forested site near Centreville, AL. ${\mathrm{NH}}_3$ mixing ratios were found to be higher at urban sites than at nearby rural (or suburban sites) except for sites which were directly influenced by local sources. Only weak correlations with temperature were observed for ${\mathrm{NH}}_3$ at the sites; slightly greater correlations were observed for total ammonia $({\mathrm{NH}}_x={\mathrm{NH}}_3+{\mathrm{NH}}_4^{+})$ vs. temperature. A weak seasonal variation was observed for ${\mathrm{NH}}_3$ mixing ratios at all sites, with all but one site exhibiting biannual maxima in spring and late summer/fall. Mean ${\mathrm{PM}}_{2.5}$ ${\mathrm{NH}}_4^{+}$ concentrations ranged from $1.78\mathrm{\mu }\mathrm{g}{\mathrm{m}}^{-3}$ in Atlanta, GA, to $1.02\mathrm{\mu }\mathrm{g}{\mathrm{m}}^{-3}$ at Oak Grove, MS, and were more uniform across the network than ${\mathrm{NH}}_3$ mixing ratios, with only slightly larger values at urban sites as compared to nearby rural (or suburban) sites. All sites exhibited highest ${\mathrm{NH}}_x$ between July and September and lowest ${\mathrm{NH}}_x$ in November and December. The gaseous ${\mathrm{NH}}_3$ fraction $({\mathrm{NH}}_3/({\mathrm{NH}}_3+{\mathrm{NH}}_4^{+}))$ was observed to decrease with increasing values of ${\mathrm{PM}}_{2.5}$ ${\mathrm{SO}}_4^{2-}$ at all sites. At two rural-forested sites and two sites near the Gulf of Mexico, the ${\mathrm{NH}}_3$ gaseous fraction approached a relatively constant value of 5–10% as ${\mathrm{PM}}_{2.5}{\mathrm{SO}}_4^{2-}$ increased beyond 5–$7\mathrm{\mu }\mathrm{g}{\mathrm{m}}^{-3}$, suggesting that ${\mathrm{NH}}_3$ availability at these locations limits aerosol neutralization.     

Characterizing Long-Term Land Use/Cover Change in the United States from 1850 to 2000 Using a Nonlinear Bi-analytical Model

We relate the historical (1850–2000) spatial and temporal changes in cropland cover in the conterminous United States to several socio-economic and biophysical determinants using an eco-region based spatial framework. Results show population density as a major determinant during the nineteenth century, and biophysical suitability as the major determinant during the twentieth century. We further examine the role of technological innovations, socio-economic and socio-ecological feedbacks that have either sustained or altered the cropland trajectories in different eco-regions. The cropland trajectories for each of the 84 level-III eco-regions were analyzed using a nonlinear bi-analytical model. In the Eastern United States, low biophysically suitable eco-regions, e.g., New England, have shown continual decline in the cropland after reaching peak levels. The cropland trajectories in high biophysically suitable regions, e.g., Corn Belt, have stabilized after reaching peak levels. In the Western United States, low-intensity crop cover (<10 %) is sustained with irrigation support. A slower rate of land conversion was found in the industrial period. Significant effect of Conservation Reserve Program on planted crop area is found in last two decades (1990–2010).     

Globalization and multi-spatial trends in the coverage of protected-area conservation (1980-2000)

This study is focused on the global expansion of protected-area coverage that occurred during the 1980--2000 period. We examine the multi-scale patterning of four of the basic facets of this expansion: i) estimated increases at the world-regional and country-level scales of total protected-area coverage; ii) transboundary protected areas; iii) conservation corridor projects; and iv) type of conservation management. Geospatial patterning of protected-area designations is a reflection of the priorities of global conservation organizations and the globalization of post-Cold War political and economic arrangements. Local and national-level factors (political leadership and infrastructure) as well as international relations such as multilateral and bilateral aid combine with these globalization processes to impact the extent, type, and location of protected-area designations. We conclude that the interaction of these factors led to the creation and reinforcement of marked spatial differences (rather than tendencies toward worldwide evenness or homogenization) in the course of protected-area expansion during the 1980--2000 period.     

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

Abstract

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

Dibenzo-p-dioxins in the environment from ceramics and pottery produced from ball clay mined in the United States

Processed ball clay samples used in the production of ceramics and samples of the ceramic products were collected and analyzed for the presence and concentration of the 2,3,7,8-Cl substituted polychlorinated dibenzo-p-dioxins and -furans (PCDDs/PCDFs). The processed ball clay had average PCDD concentrations of 3.2 ng/g toxic equivalents, a congener profile, and isomer distribution consistent with those found previously in raw ball clay. The PCDF concentrations were below the average limit of detection (LOD) of 0.5 pg/g. The final fired ceramic products were found to be free of PCDDs/PCDFs at the LODs. A consideration of the conditions involved in the firing process suggests that the PCDDs, if not destroyed, may be released to the atmosphere and could represent an as yet unidentified source of dioxins to the environment. In addition, the PCDDs in clay dust generated during manufacturing operations may represent a potential occupational exposure.     

Concentrations of polychlorinated dibenzo-p-dioxins in processed ball clay from the United States

Processed ball clays commonly used by the ceramic art industry in the United States were collected from retail suppliers and analyzed for the presence and concentration of the 2,3,7,8-Cl substituted polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/PCDFs). The average PCDD toxic equivalent (TEQ) concentrations of these processed ball clays was approximately 800 pg/g (TEQ-WHO) with characteristic congener profiles and isomer distributions similar to patterns of previously analyzed raw and processed ball clays. The PCDF concentrations were below the average limit of detection (LOD) of 0.5 pg/g. Correlation analyses reveal no significant relationship between total organic carbon (TOC) and either individual, homologues, and total tetra-through octa-chlorinated PCDD congeners, or TEQ concentrations of the processed ball clays. The results are consistent with earlier studies on levels of PCDDs in ball clays. Data from earlier studies indicated that dioxins may be released to the environment during the processing of raw clay or the firing process used in commercial ceramic facilities. The presence of dioxin in the clays also raises concerns about potential occupational exposure for individuals involved in the mining/processing of ball clay, ceramics manufacturing and ceramic artwork.     

Future land use and land cover influences on regional biogenic emissions and air quality in the United States

A regional modeling system was applied with inputs from global climate and chemistry models to quantify the effects of global change on future biogenic emissions and their impacts on ozone and biogenic secondary organic aerosols (BSOA) in the US. Biogenic emissions in the future are influenced by projected changes in global and regional climates and by variations in future land use and land cover (LULC). The modeling system was applied for five summer months for the present-day case (1990–1999, Case 1) and three future cases covering 2045–2054. Individual future cases were: present-day LULC (Case 2); projected-future LULC (Case 3); and future LULC with designated regions of tree planting for carbon sequestration (Case 4). Results showed changing future meteorology with present-day LULC (Case 2) increased average isoprene and monoterpene emission rates by 26% and 20% due to higher temperature and solar insolation. However when LULC was changed together with climate (Case 3), predicted isoprene and monoterpene emissions decreased by 52% and 31%, respectively, due primarily to projected cropland expansion. The reduction was less, at 31% and 14% respectively, when future LULC changes were accompanied by regions of tree planting (Case 4). Despite the large decrease in biogenic emission, future average daily maximum 8-h (DM8H) ozone was found to increase between +8 ppbv and +10 ppbv due to high future anthropogenic emissions and global chemistry conditions. Among the future cases, changing LULC resulted in spatially varying future ozone differences of ?5 ppbv to +5 ppbv when compared with present-day case. Future BSOA changed directly with the estimated monoterpene emissions. BSOA increased by 8% with current LULC (Case 2) but decreased by 45%–28% due to future LULC changes. Overall, the results demonstrated that on a regional basis, changes in LULC can offset temperature driven increases in biogenic emissions, and, thus, LULC projection is an important factor to consider in the study of future regional air quality.     

Biogenic Sulfur Gas Emissions from Soils in Eastern and Southeastern United States

Data are presented for the first systematic measurements of biogenic sulfur gas flux from the major soil orders within the eastern and southeastern United States. Sulfur flux samples were collected and analyzed on-site during the fall of 1977, spring and summer of 1978 and summer of 1979. A total of 27 sampling locales in 17 states were examined. Eight additional sites were visited in 1980.

At some locales, two to four soils were examined, providing an even broader sampling of the soil orders. Three of the locales were revisited two or three times during the course of the study to establish the influence of seasonal climatology upon the measured emission rates and chemical composition of the sulfur flux mixtures.

The sulfur gas enhancement of sulfur-free sweep air passing through dynamic emission flux chambers placed over selected sampling areas was determined by combined cryogenic enrichment sampling and wall-coated, open tubular, capillary column, cryogenic gas chromatography (WCOT/GC) using a sulfur selective, flame photometric detector (FPD).

Sulfur gas mixtures varied with soil order, ambient temperature, insolation, soil moisture, cultivation, and vegetative cover. Statistical analyses indicated strong temperature and soil order relationships for sulfur emissions from soils.

Fluxes ranged from 0.001 g to 1940 g of total sulfur as S/m²/yr. The calculated mean annual sulfur flux, weighted by soil order, was 0.03 g S/m²/yr for the study land area, or 110,872 metric tons (mT). The estimated annual average sulfur flux increased from 65 mT per 6400 km² for the land grids in the northernmost east-west grid tier to an average 1800 mT for the land grids in the southern Florida grid tiers.

This systematic sampling of major soils provides a much broader data base for estimating biogenic sulfur flux than previously reported for isolated intertidal sites, and presents the first sulfur flux estimates for inland soils which make up approximately 93% of the land of the eastern United States.     

An improved inventory of methane emissions from coal mining in the United States

Past efforts to estimate methane emissions from underground mines, surface mines, and other coal mine operations have been hampered, to different degrees, by a lack of direct emissions data. Direct measurements have been completely unavailable for several important coal mining operations. A primary goal of this study was to collect new methane emissions measurements and other data for the most poorly characterized mining operations and use these data to develop an improved methane emission inventory for the U.S. coal mining industry. This required the development and verification of measurement methods for surface mines, coal handling operations, and abandoned underground mines and the use of these methods at about 30 mining sites across the United States. Although the study's focus was on surface mines, abandoned underground mines, and coal handling operations, evaluations were also conducted to improve our understanding of underground mine emission trends and to develop improved national data sets of coal properties. Total U.S. methane emissions are estimated to be 4.669 million tons, and as expected, emissions from underground mine ventilation and methane drainage systems dominate (74% of the total emissions). On the other hand, emissions from coal handling, abandoned underground mines, and surface mines are significant, and collectively they represent approximately 26% of the total emissions.     

Air Pollution Emissions from Increased Industrial Coal Use in the Northeastern United States

Evaluating the air pollution impacts of energy use in the industrial sector is difficult because of the diversity and multiplicity of sources and a general lack of systematic, up-to-date data collection mechanisms. Fuel-specific energy consumption for a multi-state region is provided by the U.S. Department of Energy PIES model for a base year (1975), together with scenarios for future years. A computer model developed in this study—the Sub-regional Energy and Emissions Model (SEEM)—is applied to disaggregate the regional industrial figures to the county level according to fuel type and industrial category at the two-digit SIC level. The resulting emissions of total suspended particulates (TSP) and sulfur dioxide (SO₂) for all industrial categories are estimated at the county level by Incorporating county-specific air pollution regulations in SEEM, and are then aggregated to larger geographical regions. The model has been applied to evaluate the increased air pollution impacts of industrial energy use in the northeastern United States for two alternative 1990 scenarios: (1) the midrange/trendlong PIES projections, and (2) a Coal Replacement Scenario, which assumes a higher percentage of fuel burned in new boilers will be coal. The results are discussed in terms of implications for air pollution control policy.     

An Improved Inventory of Methane Emissions from Coal Mining in the United States

ABSTRACT

Past efforts to estimate methane emissions from underground mines, surface mines, and other coal mine operations have been hampered, to different degrees, by a lack of direct emissions data. Direct measurements have been completely unavailable for several important coal mining operations. A primary goal of this study was to collect new methane emissions measurements and other data for the most poorly characterized mining operations and use these data to develop an improved methane emission inventory for the U.S. coal mining industry. This required the development and verification of measurement methods for surface mines, coal handling operations, and abandoned underground mines and the use of these methods at about 30 mining sites across the United States. Although the study's focus was on surface mines, abandoned underground mines, and coal handling operations, evaluations were also conducted to improve our understanding of underground mine emission trends and to develop improved national data sets of coal properties. Total U.S.     

Regulating manure application discharges from concentrated animal feeding operations in the United States

In the United States, reducing pollution from agriculture has received attention due to data suggesting that this is the leading source of impairment of many waterbodies. The federal government revised its regulations governing concentrated animal feeding operations (CAFOs) to enhance governmental oversight over sources of pollution. For the application of manure resulting in pollutant discharges, CAFOs need to implement nutrient management plans. A federal court affirmed the ability of the US federal government to oversee the application of manure from CAFOs that have discharges. Simultaneously, owners and operators of CAFOs who have implemented an appropriate nutrient management plan may forgo securing a permit if their discharges qualify under the agricultural stormwater discharge exemption.     

A survey of polycyclic musks in selected household commodities from the United States

Occurrence of the polycyclic musks, 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronapthalene (AHTN), in wastewater influent and effluent, as well as in surface waters, has been reported. HHCB and AHTN were also reported to occur in human and wildlife tissues. The major sources for HHCB and AHTN to wastewater are thought to be consumer products such as shampoos, deodorants, laundry detergents, and household surface cleaners. However, the levels of HHCB and AHTN in consumer products are not known. For evaluation of the sources of human and environmental exposures, characterization of levels of HHCB and AHTN in consumer products is needed. In this study, we measured concentrations of HHCB (Galaxolide), AHTN (Tonalide), and HHCB-lactone (Galaxolidone) from a variety of consumer products, including perfumes, body lotions, and deodorants. Concentrations of HHCB, AHTN, and HHCB-lactone in consumer products ranged from <5 ng/g to over 4000 microg/g, <5 ng/g to 451 microg/g, and <5 ng/g to 217 microg/g, respectively. The highest concentrations were found in perfumes, body creams and lotions, and deodorants. The results suggest that a wide variety of source materials exist for HHCB and AHTN, and that these materials are used on a daily basis.     

Dibenzo-p-dioxins in the environment from ceramics and pottery produced from ball clay mined in the United States

Processed ball clay samples used in the production of ceramics and samples of the ceramic products were collected and analyzed for the presence and concentration of the 2,3,7,8-Cl substituted polychlorinated dibenzo-p-dioxins and -furans (PCDDs/PCDFs). The processed ball clay had average PCDD concentrations of 3.2 ng/g toxic equivalents, a congener profile, and isomer distribution consistent with those found previously in raw ball clay. The PCDF concentrations were below the average limit of detection (LOD) of 0.5 pg/g. The final fired ceramic products were found to be free of PCDDs/PCDFs at the LODs. A consideration of the conditions involved in the firing process suggests that the PCDDs, if not destroyed, may be released to the atmosphere and could represent an as yet unidentified source of dioxins to the environment. In addition, the PCDDs in clay dust generated during manufacturing operations may represent a potential occupational exposure.     

Temporal trends (1990-2000) in the concentration of cadmium, lead and mercury in mosses across Europe

The European heavy metals in mosses survey provides data on the concentration of 10 heavy metals in naturally growing mosses. The survey has been repeated at five-yearly intervals and in this paper we report on the temporal trends in the concentration of cadmium, lead and mercury between 1990 and 2000. Metal- and country-specific temporal trends were observed. In general, the concentration of lead and cadmium in mosses decreased between 1990 and 2000; the decline was higher for lead than cadmium. For mercury not enough data were available to establish temporal trends between 1990 and 1995, but between 1995 and 2000 the mercury concentration in mosses did not change across Europe. The observed temporal trends for the concentrations in mosses were similar to the trends reported for the modelled total deposition of cadmium, lead and mercury in Europe.     

Polycyclic musk compounds in higher trophic level aquatic organisms and humans from the United States

Polycyclic musks, 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronaphthalene (AHTN), are used as fragrance ingredients in numerous consumer products such as cleaning agents and personal care products. Studies have reported the widespread occurrence of these musks in surface waters and fish from western European countries. Nevertheless, little is known about their accumulation in humans and wildlife in the United States. In this study, we measured concentrations of HHCB and AHTN in human adipose fat collected from New York City. Furthermore, tissues from marine mammals, water birds, and fish collected from US waters were analyzed to determine the concentrations of HHCB and AHTN. Concentrations of HHCB and AHTN in human adipose fat samples ranged from 12 to 798 and from <5 to 134 ng/g, on a lipid weight basis, respectively. A significant correlation existed between the concentrations of HHCB and AHTN in human adipose fat. Concentrations of HHCB and AHTN were not positively correlated with age or gender of the donors. HHCB was found in tissues of several wildlife species, but not in the livers of polar bear from the Alaskan Arctic. Among wildlife species analyzed, spinner and bottlenose dolphins collected from Florida coastal waters contained measurable concentrations of HHCB.