Trends Network Sites Research Articles

A Measurement-Model Fusion Approach for Improved Wet Deposition Maps and Trends.

Air quality models provide spatial fields of wet deposition (WD) and dry deposition that explicitly account for the transport and transformation of emissions from thousands of sources. However, many sources of uncertainty in the air quality model including errors in emissions and meteorological inputs (particularly precipitation) and incomplete descriptions of the chemical and physical processes governing deposition can lead to bias and error in the simulation of WD. We present an approach to bias correct Community Multiscale Air Quality model output over the contiguous United States using observation‐based gridded precipitation data generated by the Parameter‐elevation Regressions on Independent Slopes Model and WD observations at the National Atmospheric Deposition Program National Trends Network sites. A cross‐validation analysis shows that the adjusted annual accumulated WD for NO3 −, NH4 +, and SO4 2− from 2002 to 2012 has less bias and higher correlation with observed values than the base model output without adjustment. Temporal trends in observed WD are captured well by the adjusted model simulations across the entire contiguous United States. Consistent with previous trend analyses, WD NO3 − and SO4 2− are shown to decrease during this period in the eastern half of the United States, particularly in the Northeast, while remaining nearly constant in the West. Trends in WD of NH4 + are more spatially and temporally heterogeneous, with some positive trends in the Great Plains and Central Valley of CA and slightly negative trends in the south.

Seasonal Patterns of Dry Deposition at a High‐Elevation Site in the Colorado Rocky Mountains

AbstractIn the Colorado Rocky Mountains, high‐elevation barren soils are deficient in carbon (C) and phosphorus (P) and enriched in nitrogen (N). The seasonal variability of dry deposition and its contributions to alpine elemental budgets is critical to understanding how dry deposition influences biogeochemical cycling in high‐elevation environments. In this 2 year study, we evaluated dry and wet deposition inputs to the Niwot Ridge Long Term Ecological Research (NWT LTER) site in the Colorado Rocky Mountains. The total organic C flux in wet + dry (including soluble and particulate C) deposition was >30 kg C ha−1 yr−1 and represents a substantial input for this C‐limited environment. Our side‐by‐side comparison of dry deposition collectors with and without marble insert indicated that the insert improved retention of dry deposition by ~28%. Annual average dry deposition fluxes of water‐soluble organic carbon (4.25 kg C ha−1 yr−1) and other water‐soluble constituents, including ammonium (0.16 kg NH4+ha−1 yr−1), nitrate (1.99 kg NO3− ha−1 yr−1), phosphate (0.08 kg PO43− ha−1 yr−1), and sulfate (1.20 kg SO42− ha−1 yr−1), were comparable to those in wet deposition, with highest values measured in the summer. Backward trajectory analyses implicate air masses passing through the arid west and Four Corners, USA, as dominant source areas for dry deposition, especially in spring months. Synchronous temporal patterns of deposition observed at the NWT LTER site and a distant Rocky Mountain National Park Clean Air Status and Trends Network site indicate that seasonal dry deposition patterns are regional phenomena with important implications for the larger Rocky Mountain region.

Identifying and Quantifying Phakopsora pachyrhizi Spores in Rain

In summers of 2005 and 2006, rain was collected weekly at over 100 selected National Atmospheric Deposition Program/National Trends Network sites across the soybean-growing region of the central and eastern United States. Rain samples were screened for Phakopsora pachyrhizi (causal agent of soybean rust) DNA using a nested real-time polymerase chain reaction assay. Over this time frame, P. pachyrhizi spores were detected in every state in the study, but more frequently in states along the Gulf and Atlantic coasts and along the Ohio River Valley westward to Kansas. A bimodal temporal distribution of samples testing positive for P. pachyrhizi was found in both years. However, there was a greater than threefold increase in the number of samples testing positive for P. pachyrhizi in 2006 compared with 2005, with the most significant increase in August. There was also an increase in the average number of spores per sample in 2006 relative to 2005. Sequence analysis of a subset of positive samples was used to validate the assay results. From the sequence analysis, two reliable polymorphic regions were found, resulting in six distinct genotypes. One genotype was found in 56% of the samples tested, whereas the other genotypes were found less frequently.

Source Apportionment of Airborne Particulate Matter for the Speciation Trends Network Site in Cleveland, OH

Aerosol composition data from the Speciation Trends Network (STN) site (East 14th Street) in Cleveland, OH, were analyzed by advanced receptor model methods for source apportionment as well as by the standard positive matrix factorization (PMF) using PMF2. These different models are used in combination to test model limitations. These data were 24-hr average mass concentrations and compositions obtained for samples taken every third day from 2001 to 2003. The Multilinear Engine (ME) was used to solve an expanded model to estimate the source profiles and source contributions and also to investigate the wind speed, wind direction, time-of-day, weekend/weekday, and seasonal effects. PMF2 was applied to the same data-set. Potential source contribution function (PSCF) and conditional probability function (CPF) analyses were used to locate the regional and local sources using the resolved source contributions and appropriate meteorological data. Very little difference was observed between the results of the expanded model and the PMF2 values for the profiles and source contribution time series. The identified sources were as ferrous smelter, secondary sulfate, secondary nitrate, soil/combustion mixture, steel mill, traffic, wood smoke, and coal burning. The CPF analysis was useful in helping to identify local sources, whereas the PSCF results were only useful for regional source areas. Both of these analyses were more useful than the wind directional factor derived from the expanded factor analysis. However, the expanded analysis provided direct information on seasonality and day-of-week behavior of the sources.

Supplemental Material for Source Apportionment of Airborne Particulate Matter for the Speciation Trends Network Sites in Cleveland, Oh

Supplemental Material for Source Apportionment of Airborne Particulate Matter for the Speciation Trends Network Sites in Cleveland, Oh

Fine Particulate Matter Source Apportionment for the Chemical Speciation Trends Network Site at Birmingham, Alabama, Using Positive Matrix Factorization

The Positive Matrix Factorization (PMF) receptor model version 1.1 was used with data from the fine particulate matter (PM2.5) Chemical Speciation Trends Network (STN) to estimate source contributions to ambient PM2.5 in a highly industrialized urban setting in the southeastern United States. Model results consistently resolved 10 factors that are interpreted as two secondary, five industrial, one motor vehicle, one road dust, and one biomass burning sources. The STN dataset is generally not corrected for field blank levels, which are significant in the case of organic carbon (OC). Estimation of primary OC using the elemental carbon (EC) tracer method applied on a seasonal basis significantly improved the model’s performance. Uniform increase of input data uncertainty and exclusion of a few outlier samples (associated with high potassium) further improved the model results. However, it was found that most PMF factors did not cleanly represent single source types and instead are “contaminated” by other sources, a situation that might be improved by controlling rotational ambiguity within the model. Secondary particulate matter formed by atmospheric processes, such as sulfate and secondary OC, contribute the majority of ambient PM2.5 and exhibit strong seasonality (37 ± 10% winter vs. 55 ± 16% summer average). Motor vehicle emissions constitute the biggest primary PM2.5 mass contribution with almost 25 ± 2% long-term average and winter maximum of 29 ± 11%. PM2.5 contributions from the five identified industrial sources vary little with season and average 14 ± 1.3%. In summary, this study demonstrates the utility of the EC tracer method to effectively blank-correct the OC concentrations in the STN dataset. In addition, examination of the effect of input uncertainty estimates on model results indicates that the estimated uncertainties currently being provided with the STN data may be somewhat lower than the levels needed for optimum modeling results.

Supplemental Material to "Fine Particulate Matter Source Apportionment for the Chemical Speciation Trends Network Site at Birmingham, Alabama, Using Positive Matrix Factorization" by Baumann et al.

Supplemental Material to "Fine Particulate Matter Source Apportionment for the Chemical Speciation Trends Network Site at Birmingham, Alabama, Using Positive Matrix Factorization" by Baumann et al.

Comparison of Source Apportionments of Fine Particulate Matter at Two San Jose Speciation Trends Network Sites

In this study, the chemical composition of fine particulate matter samples collected at U.S. Environmental Protection Agency Speciation Trends Network sites in San Jose, CA, from February 2000 to February 2005 were analyzed. A San Jose site was initially established at 4th Street and then subsequently moved to Jackson Street in mid-2002. These sites are approximately 1 km apart. There were no known major changes in the nature of the sources in the area over this period. The study used positive matrix factorization model to extract the source profiles and their mass contributions and to compare the results for the congruence of the source apportionments between these two nearby sites. In the case of the 4th Street site, the average mass was apportioned to wood combustion (32.1 +/- 2.5%), secondary nitrate (22.3 +/- 2%), secondary sulfate (10.7 +/- 0.6%), fresh sea salt (7.7 +/- 0.9%), gasoline vehicles (7.3 +/- 0.5%), aged sea salt (6.8 +/- 0.4%), road dust (6.7 +/- 0.7%), diesel emissions (3.9 +/- 0.3%), and a Ni-related industrial source (2.5 +/- 0.4%). At the Jackson Street site, the average mass was apportioned to wood combustion (33.6 +/- 2.6%), secondary nitrate (20.3 +/- 1.9%), secondary sulfate (13.9 +/- 0.9%), aged sea salt (12.4 +/- 0.7%), gasoline vehicle (8.3 +/- 0.6%), fresh sea salt (5.3 +/- 0.5%), diesel emission (3.2 +/- 0.3%), road dust (1.9 +/- 0.1%), and Ni-related industrial source (1.3 +/- 0.1%). Conditional probability function analysis was used to help identify local sources. These results suggested that moving the sampling site a short distance had little effect on the nature of the resolved source types although some differences in their quantitative impacts were obtained in the positive matrix factorization analyses.

Changes in the Chemistry of Precipitation in the United States, 1981–1998

Regulatory measures in the United States, such as Title IV of the Clean Air Act Amendments of 1990, have primarily restricted sulfur dioxide emissions as a way to control acidic deposition. These restrictions, coupled with increasing concentrations of NH4+ in wet deposition in some regions of the U.S. and continued high emissions of nitrogen oxides have generated a significant shift in the chemistry of precipitation as measured at National Atmospheric Deposition Program/National Trends Network sites. Trends in precipitation chemistry at NADP/NTN sites were evaluated for statistical significance for the period 1981–1998 using a Seasonal Mann-Kendall Test, a robust non-parametric test for detection of monotonic trends. SO42− declines were detected at 100 of the 147 sites examined while no sites exhibited increasing SO42− trends. On average, SO42− declined 35% over the period 1981–1998 with downward SO42− trends being most pronounced in the north-eastern United States. In contrast, no consistent trends in NO3− concentrations were observed in precipitation in any major region of the United States. Although the majority of sites did not exhibit significant trends in NH4+ concentration, 30 sites exhibited upward trends. For Ca2+ concentration in precipitation, 64 sites exhibited a significant decreasing trend and no sites exhibited an upward trend.

Trends in Ammonium Concentration in Precipitation and Atmospheric Ammonia Emissions at a Coastal Plain Site in North Carolina, U.S.A.

The temporal characteristics of annual volume-weighted average ammonium (NH4+) ion concentration in precipitation and local ammonia (NH3) emissions are investigated over the period 1982−1997 at National Atmospheric Deposition Program/National Trends Network site NC35, located in Sampson County, NC. Multiple regression analysis of annual volume-weighted average values of NH4+ concentration in precipitation identifies a statistically significant (p < 0.01) 4-year cycle and increasing trend during the period. The cycle is likely a function of mean annual ambient surface temperature, which is shown to be a significant (p < 0.01) predictor variable for annual NH4+ concentrations in precipitation. Loess fitting suggests that NH4+ concentration in precipitation began to increase more rapidly between 1989 and 1990. An analysis of estimated population-based annual NH3 emissions from individual sources in an intensively managed agricultural region surrounding NC35 shows that emissions from swine (p < 0.01), fertilizer (p < 0.10), turkeys (p < 0.05), and broilers (p < 0.05) are significantly greater during the period 1990−1997 than the period 1982−1989. Emissions from non-broiler chickens are significantly (p < 0.01) lower during the period 1990−1997. Cattle emissions are not significantly different (10% level) during the two periods. The increase in average annual swine emissions between periods accounts for ≈84% of the increase in average annual emissions from all sources between periods. Variability in local ammonia emissions from swine and mean ambient surface temperature explain ap proximately 90% of the variation in annual volume-weighted average NH4+ concentrations in precipitation at NC35 during the period 1982−1997.

A possible deficiency in estimates of wet deposition obtained from data generated by the NADP/NTN network

A conventional precipitation scavenging model is used to evaluate the effect of the performance of a wet-deposition collector on the reported deposition amounts. Three National Atmospheric Deposition Program/National Trends Network sites in semi arid western Colorado were chosen to evaluate chloride and sulfate wet deposition. Observations of the performance of a wet-deposition collector have demonstrated a delay in opening and cycling during a precipitation event. A significant fraction of wet deposition may be excluded when small amounts of initial precipitation are not sampled and a potentially large fraction of annual wet deposition may be excluded if a majority of precipitation events are small. The actual amount missed depends on the precipitation intensity, variability of intensity with time, raindrop or snowflake size and the individual performance characteristics of the collector. Detailed performance data are needed for individual welt-deposition collectors before accurate estimates of wet deposition can be expected.

The precision of wet atmospheric deposition data from national atmospheric deposition program/national trends network sites determined with collocated samplers

Abstract A collocated, wet-deposition sampler program has been operated since October 1988 by the U.S. Geological Survey to estimate the overall sampling precision of wet atmospheric deposition data collected at selected sites in the National Atmospheric Deposition Program and National Trends Network (NADP/NTN). A duplicate set of wet-deposition sampling instruments was installed adjacent to existing sampling instruments at four different NADP/NTN sites for each year of the study. Wet-deposition samples from collocated sites were collected and analysed using standard NADP/NTN procedures. Laboratory analyses included determinations of pH, specific conductance, and concentrations of major cations and anions. The estimates of precision included all variability in the data-collection system, from the point of sample collection through storage in the NADP, /NTN database. Sampling precision was determined from the absolute value of differences in the analytical results for the paired samples in terms of median relative and absolute difference. The median relative difference for Mg 2+ , Na + , K 4 + and NH concentration and deposition was quite variable between sites and exceeded 10% at most sites. Relative error for analytes whose concentrations typically approached laboratory method detection limits were greater than for analytes that did not typically approach detection limits. The median relative difference for S0 4 2− and NO 3 − concentration, specific conductance, and sample volume at all sites was less than 7%. Precision for H + concentration and deposition ranged from less than 10% at sites with typically high levels of H + concentration to greater than 30% at sites with low H + concentration. Median difference for analyte concentration and deposition was typically 1.5-2-times greater for samples collected during the winter than during other seasons at two northern sites. Likewise, the median relative difference in sample volume for winter samples was more than double the annual median relative difference at the two northern sites. Bias accounted for less than 25% of the collocated variability in analyte concentration and deposition from weekly collocated precipitation samples at most sites.