Application of an atmospheric tracer ratio method to estimation of PM2.5 emission rates from wheat conveying operations at a wheat pile storage facility.

Particulate matter (PM) pollution is associated with adverse effects on human health and the environment. There is no designated PM2.5 emission factor for horizontal grain conveyors. Instead, in Washington state, the air permitting agency uses an emission factor for headhouse and grain handling operations to issue permits. There is concern that this factor does not accurately represent the conveyor operations and limits the size and operation of wheat pile facilities. The primary goal of this work was to estimate the PM2.5 emission rate (which can further be converted to an emission factor) from wheat conveying operations at a large wheat pile storage facility in eastern Washington using an atmospheric tracer ratio method, with CO2 gas as the tracer. The field study results yield an emission rate of 5.2[Formula: see text]1.7 grams of PM2.5 per hour and these emissions are due to the transfer point from an upper belt to a lower belt. This rate is approximately 320 times lower than the emission rate for headhouse operations which has been used previously to represent conveyor operations. The emission rate was in relatively good agreement with results of an inverse Gaussian plume model calculation of emissions using measured ambient PM2.5 levels at a very short distance downwind of the transfer point. A consistent PM2.5 to tracer gas ratio over the tests showed that PM2.5 and CO2 disperse in a similar manner and confirmed that the CO2 tracer release was a reliable simulation of the PM2.5 pollutant source over distances involved in the study (less than 10 meters). The results also indicate a need for the Environmental Protection Agency to develop a designated PM2.5 emission factor for wheat conveyance. IMPLICATIONS: There are presently no emission factors available for large wheat pile storage facilities where wheat is transferred via long horizontal conveyor belts. As a result, local and state permitting agencies use emission factors for other types of grain handling systems. In this paper, we report the first measurements of PM2.5 emission rates (that can further be converted to emission factors using a known grain rate on the conveyor) for horizontal grain conveyors used at wheat pile storage facilities. The measured emission rate is much less than the emission rate derived from the surrogate emission factor currently used for permit purposes. This has implications for the size and operation of wheat pile storage facilities.

Methoxyphenols and levoglucosan ratios in PM2.5 from wheat and Kentucky bluegrass stubble burning in eastern Washington and northern Idaho.

Eastern Washington is compromised by various pollution sources, of which agricultural burning is a particular burden. Smoke from field burning is a nuisance to nearby communities and is a concern for health. This study evaluates levoglucosan (LG) and methoxyphenols (MPs) as potential tracers for apportioning field burning smoke. PM2.5 (particulate matter < 2.5 microM m in aerodynamic diameter) samples from wheat and Kentucky bluegrass (KBG) stubble smoke were collected from chamber and field burns. The samples were analyzed for inorganic and organic tracers, including LG and 19 MPs. For the chamber experiments, the amount of LG, approximately 23 microg mg(-1) PM2.5, found in wheat and KBG stubble smoke was similar, while the total MPs was higher in wheat. Trace elements associated with soil were found in smoke samples in the field. Syringaldehyde, acetosyringone, and coniferylaldehyde were found to be the most prominent particle-phase MPs in wheat smoke, and these compounds were not always present in detectable amounts in KBG smoke. The ratio of LG/ syringaldehyde found in wheat (78 +/- 27) was higher than the same ratio reported for softwoods (22 +/- 3) and hardwoods (approximately 5). Similarly, the ratio of LG/coniferylaidehyde was higher in wheat stubble smoke (180 +/- 39) compared to that in softwoods (approximately 7) and hardwoods (approximately 8).

Loading effect correction for real-time aethalometer measurements of fresh diesel soot.

In this study, a correction was developed for the aethalometer to measure real-time black carbon (BC) concentrations in an environment dominated by fresh diesel soot. The relationship between the actual mass-specific absorption coefficient for BC and the BC-dependent attenuation coefficients was determined from experiments conducted in a diesel exposure chamber that provided constant concentrations of fine particulate matter (PM; PM(2.5); PM < 2.5 microm in aerodynamic diameter) from diesel exhaust. The aethalometer reported BC concentrations decreasing with time from 48.1 to 31.5 microg m(-3) when exposed to constant PM(2.5) concentrations of 55 +/- 1 microg m(-3) and b(scat) = 95 +/- 3 Mm(-1) from diesel exhaust. This apparent decrease in reported light-absorbing PM concentration was used to derive a correction K(ATN) for loading of strong light-absorbing particles onto or into the aethalometer filter tape, which was a function of attenuation of light at 880 nm by the embedded particles.

Ambient woodsmoke and associated respiratory emergency department visits in Spokane, Washington.

Three multivariate receptor algorithms were applied to seven years of chemical speciation data to apportion fine particulate matter to various sources in Spokane, Washington. Source marker compounds were used to assess the associations between atmospheric concentration of these compounds and daily cardiac hospital admissions and/or respiratory emergency department visits. Total carbon and arsenic had high correlations with two different vegetative burning sources and were selected as vegetative burning markers, while zinc and silicon were selected as markers for the motor vehicle and airborne soil sources, respectively. The rate of respiratory emergency department visits increased 2% for a 3.0 microg/m3 interquartile range change in a vegetative burning source marker (1.023, 95% CI 1.009-1.038) at a lag of one day. The other source markers studied were not associated with the health outcomes investigated. Results suggest vegetative burning is associated with acute respiratory events.

Modeling ozone and aerosol formation and transport in the pacific northwest with the community Multi-Scale Air Quality (CMAQ) modeling system.

The Community Multi-Scale Air Quality (CMAQ) modeling system was used to investigate ozone and aerosol concentrations in the Pacific Northwest (PNW) during hot summertime conditions during July 1-15, 1996. Two emission inventories (El) were developed: emissions for the first El were based upon the National Emission Trend 1996 (NET96) database and the BEIS2 biogenic emission model, and emissions for the second El were developed through a "bottom up" approach that included biogenic emissions obtained from the GLOBEIS model. The two simulations showed that elevated PM2.5 concentrations occurred near and downwind of the Interstate-5 corridor along the foothills of the Cascade Mountains and in forested areas of central Idaho. The relative contributions of organic and inorganic aerosols varied by region, but generally organic aerosols constituted the largest fraction of PM2.5. In wilderness areas near the 1-5 corridor, organic carbon from anthropogenic sources contributed approximately 50% of the total organic carbon with the remainder from biogenic precursors, while in wilderness areas in Idaho, biogenic organic carbon accounted for 80% of the total organic aerosol. Regional analysis of the secondary organic aerosol formation in the Columbia River Gorge, Central Idaho, and the Olympics/Puget Sound showed that the production rate of secondary organic carbon depends on local terpene concentrations and the local oxidizing capacity of the atmosphere, which was strongly influenced by anthropogenic emissions. Comparison with observations from 12 IMPROVE sites and 21 ozone monitoring sites showed that results from the two El simulations generally bracketed the average observed PM parameters and that errors calculated for the model results were within acceptable bounds. Analysis across all statistical parameters indicated that the NW-AIRQUEST El solution performed better at predicting PM2.5, PM1, and beta(ext) even though organic carbon PM was over-predicted, and the NET96 El solution performed better with regard to the inorganic aerosols. For the NW-AIRQUEST El solution, the normalized bias was 30% and the normalized absolute error was 49% for PM2.5 mass. The NW-AIRQUEST solution slightly overestimated peak hourly ozone downwind of urban areas, while the NET96 solution slightly underestimated peak values, and both solutions over-predicted average 03 concentrations across the domain by approximately 6 ppb.

Association between particulate matter and emergency room visits, hospital admissions and mortality in Spokane, Washington.

There is conflicting evidence regarding the association between different size fractions of particulate matter (PM) and cardiac and respiratory morbidity and mortality. We investigated the short-term associations of four size fractions of particulate matter (PM(1), PM(2.5), PM(10), and PM(10-2.5)) and carbon monoxide with hospital admissions and emergency room (ER) visits for respiratory and cardiac conditions and mortality in Spokane, Washington. We used a log-linear generalized linear model to compare daily averages of PM and carbon monoxide with daily counts of the morbidity and mortality outcomes from January 1995 to June 2001. We examined pollution lags ranging from 0 to 3 days and compared our results to a similar log-linear generalized additive model. Effect estimates tended to be smaller and have larger standard errors for the generalized linear model. Overall, we saw no association with respiratory ER visits and any size fraction of PM. However, there was a suggestion of greater respiratory effect from fine PM when compared to coarse fraction. Carbon monoxide was associated with both all respiratory ER visits and visits for asthma at the 3-day lag. We feel that carbon monoxide may be serving as a marker for combustion-derived pollutants, which is one large component of the diverse air pollutant mixture. We also found no association with any size fraction of PM or CO with cardiac hospital admissions or mortality at the 0- to 3-day lag. We found no consistent associations between any size fraction of PM and cardiac or respiratory ER visits or hospital admissions.

An analysis of the association between respiratory symptoms in subjects with asthma and daily air pollution in Spokane, Washington.

The association between respiratory symptoms and ambient levels of particulate matter (PM) air pollution has been the focus of several panel studies. The majority of studies focused only on PM10, were conducted for relatively short periods, reported peak flow data, and involved children with asthma. The goal of our study was to evaluate the effect of particulate matter of various size fractions (PM10, PM2.5, PM1.0, and PM coarse fraction) on respiratory symptoms in both adults and children with asthma monitored over many months. Daily diary data on respiratory symptoms and medication use were collected. Air pollution data were collected by the local air agency and Washington State University. Data were collected in Spokane, WA, a semiarid city with diverse sources of particulate matter, including motor vehicles, woodstoves, agricultural burning, resuspended road dust, and dust storms. Sixteen adults and nine children living in Spokane participated in the study. The majority of adult subjects participated for over 1 yr and the children were studied for over 8 mo. In the children, we found a strong association between cough and PM10, PM2.5, PM coarse fraction, and PM1.0(p < .05). Sputum production and runny nose were associated with PM10and coarse fraction. However, no association was found between the presence of any respiratory symptom any PM metric in the adult subjects. These positive associations between various metrics of PM and respiratory symptoms in children suggest that children are more sensitive than adults to the effects of increased levels of PM air pollution or that the central site monitor was more representative for children who spend more time outdoors than adults. These findings also suggest that both larger and smaller particles can aggravate asthma symptoms.

Source apportionment of indoor, outdoor, and personal PM2.5 in Seattle, Washington, using positive matrix factorization.

As part of a large exposure assessment and health-effects panel study, 33 trace elements and light-absorbing carbon were measured on 24-hr fixed-site filter samples for particulate matter with an aerodynamic diameter <2.5 microm (PM2.5) collected between September 26, 2000, and May 25, 2001, at a central outdoor site, immediately outside each subject's residence, inside each residence, and on each subject (personal sample). Both two-way (PMF2) and three-way (PMF3) positive matrix factorization were used to deduce the sources contributing to PM2.5. Five sources contributing to the indoor and outdoor samples were identified: vegetative burning, mobile emissions, secondary sulfate, a source rich in chlorine, and a source of crustal-derived material. Vegetative burning contributed more PM2.5 mass on average than any other source in all microenvironments, with average values estimated by PMF2 and PMF3, respectively, of 7.6 and 8.7 microg/m3 for the outdoor samples, 4 and 5.3 microg/m3 for the indoor samples, and 3.8 and 3.4 microg/m3 for the personal samples. Personal exposure to the combustion-related particles was correlated with outdoor sources, whereas exposure to the crustal and chlorine-rich particles was not. Personal exposures to crustal sources were strongly associated with personal activities, especially time spent at school among the child subjects.

Monitoring of particulate matter outdoors.

Recent studies of the size and composition of atmospheric particulate matter (PM) have demonstrated the usefulness of separating atmospheric PM into its fine and coarse components. The need to measure the mass and composition of fine and coarse PM separately has been emphasized by research in exposure, epidemiology, and toxicology of atmospheric PM. This paper provides a background on the size distribution and properties of PM relevant to the differences between fine and coarse particles. Various decisions that must be made when deciding how to separate, collect, and measure PM are discussed. Techniques for monitoring fine and coarse particles, including the US Federal Reference Method for PM2.5 and several techniques for PM10-2.5, are presented. Problems encountered in collecting semivolatile PM and in weighing atmospheric PM collected on a filter are described. Continuous monitoring methods for PM mass and for PM components (carbon, nitrate, and sulfate) are described and brief descriptions are given of analytical techniques for the chemical characterization of collected PM. This information should be especially useful for environmental workers familiar with monitoring methods for total suspended particles or PM10 but who will need to measure PM2, and PM10-2.5 in the future.

Testing the metals hypothesis in Spokane, Washington.

A >7-year, time-series, epidemiologic study is ongoing in Spokane, Washington, to examine the associations between ambient particulate constituents or sources and health outcomes such as emergency department (ED) visits for asthma or respiratory problems. One of the hypotheses being tested is that particulate toxic metals are associated with these health outcomes. Spokane is a desirable city in which to conduct this study because of its relatively high concentrations of particulate matter, low concentrations of potentially confounding air pollutants, variability of particulate sources, and presence of several potential particulate metals sources. Daily fine- and coarse-fraction particulate samples are analyzed for metals via energy-dispersive X-ray fluorescence (EDXRF) and instrumental neutron activation analysis. Particulate sources are determined using receptor modeling, including chemical mass balancing and positive matrix factorization coupled with partial source contribution function analysis. Principal component analysis has also been used to examine the influence of sources on the daily variability of the chemical composition of particulate samples. Based upon initial analyses using the EDXRF elemental analyses, statistically significant associations were observed between ED visits for asthma and increased combustion products, air stagnation, and fine particulate Zn. Although there is a significant soil particulate component, increased crustal particulate levels were not found to be associated with ED visits for asthma. Further research will clarify whether there is an association between specific health outcomes and either coarse or fine particulate metal species.

Development and evaluation of a personal particulate organic and mass sampler.

Accurate measurement of personal exposure to particulate matter and its constituents requires samplers that are accurate, compact, lightweight, inexpensive, and convenient to use. The personal particulate organic and mass sampler (PPOMS) has been developed to meet these criteria. The PPOMS uses activated carbon-impregnated foam as a combined 2.5-microm size-selective inlet and denuder for assessment of fine particle mass and organic carbon. Proof of the PPOMS concept has been established by comparing mass and organic carbon in particles collected with collocated samplers in Seattle, at a central outdoor site, and in residences. Daily particulate mass concentrations averaged 10.0 +/- 5.2, 12.0 +/- 5.3, and 11.2 +/- 5.1 microg m(-3) for the Federal Reference Method, the Harvard Personal Exposure Monitor, and the PPOMS, respectively, for 10 24-h sampling periods. During a series of PM2.5 indoor organic carbon (OC) measurements from single quartz filters, the apparent indoor OC averaged 7.7 +/- 0.8 microg of C m(-3), which was close to the indoor PM2.5 mass from collocated Teflon filters (7.3 +/- 2.3 microg of C m(-3)), indicating the presence of a large positive OC artifact. In collocated measurements, the PPOMS eliminated this artifact just as well as the integrated gas and particle sampler that incorporated a macroreticular polystyrene-divinylbenzene (XAD-4) resin-coated denuder, yielding OC concentrations of 2.5 +/- 0.4 and 2.4 +/- 1.0 microg of C m(-3), respectively. Thermal analysis for OC indicated that the indoor positive artifact was due to adsorption of gas-phase semivolatile organic compounds (SVOC). This study shows that the PPOMS design provides a 2.5-microm size-selective inlet that also prevents the adsorption of gas-phase SVOC onto quartz filters, thus eliminating the filter positive artifact The PPOMS meets a significant current challenge for indoor and personal sampling of particulate organic carbon. The PPOMS design can also simplify accurate ambient sampling for PM2.5.