Jack M. Wolfson

Long-term measurements of respirable sulfates and particles inside and outside homes

The results of extensive indoor and outdoor monitoring for respirable size particles and the sulfate fraction of these particles are reported. These air pollution measurements were obtained in conjunction with an epidemiologic study in six U.S. cities: Portage, Wisconsin; Topeka, Kansas; Kingston/Harriman, Tennessee; Watertown, Massachusetts; St. Louis, Missouri: and Steubenville, Ohio. The major source of indoor particulate matter is cigarette smoke, which contributes approximately 20 μm−3 to the indoor concentrations for each smoker. Even in homes without smokers, indoor particle concentrations equal or exceed outdoor levels. The indoor respirable sulfate concentrations are consistently lower than outdoor concentrations.

Evaluation of an annular denuder/filter pack system to collect acidic aerosols and gases

A glass impactor was designed and evaluated along with an annular denude/filter pack system. The glass impactor has a 50% aerodynamic cutoff of 2.1 ..mu..m at a flow of 10 L min/sup /minus/1/ and allows a quantitative transfer of gases and fine particles to the annular denuder and filter pack components. Fine particle and gas concentrations, determined by using the glass impactor along with the annular denuder/filter pack, were in good agreement with those obtained with colocated reference samplers. Measurements of SO/sub 2/, HNO/sub 3/, and HNO/sub 2/ gases showed mean collection efficiencies of 0.993, 0.984, and 0.952, respectively, which compare well with predicted values. Additionally, it was found that artifact formation of nitrate and nitrite ions, representing about 5-10% of the concentrations of HNO/sub 3/ and HNO/sub 2/, occurs in the Na/sub 2/CO/sub 3/-coated annular denuder. Corrections for these artifacts were made with a second Na/sub 2/CO/sub 3/-coated annular denuder. The results of this pilot study suggest that the glass impactor/annular denuder/filter pack sampling system is suitable for measuring acidic aerosols and gases.

An improved method for measuring aerosol strong acidity: Results from a nine-month study in St Louis, Missouri and Kingston, Tennessee

Abstract An improved method for measuring strong acidity of atmospheric aerosols is presented. An ammonia diffusion denuder was developed to prevent neutralization of the acidic aerosol samples. In addition, a new procedure for protecting samples during shipment and analysis was used. An increase in the sensitivity of the analysis was achieved by extraction of the aerosol sample in a small solution volume, 3 ml, of 10−4 N HClO4, and the use of a microelectrode for pH determination. Finally, results from a nine-month study in St Louis, Missouri and Kingston, Tennessee are given.

Indoor, outdoor, and regional summer and winter concentrations of PM10, PM2.5, SO4(2)-, H+, NH4+, NO3-, NH3, and nitrous acid in homes with and without kerosene space heaters.

Twenty-four-hour samples of PM10 (mass of particles with aerodynamic diameter < or = 10 microm), PM2.5, (mass of particles with aerodynamic diameter < or = 2.5 microm), particle strong acidity (H+), sulfate (SO42-), nitrate (NO3-), ammonia (NH3), nitrous acid (HONO), and sulfur dioxide were collected inside and outside of 281 homes during winter and summer periods. Measurements were also conducted during summer periods at a regional site. A total of 58 homes of nonsmokers were sampled during the summer periods and 223 homes were sampled during the winter periods. Seventy-four of the homes sampled during the winter reported the use of a kerosene heater. All homes sampled in the summer were located in southwest Virginia. All but 20 homes sampled in the winter were also located in southwest Virginia; the remainder of the homes were located in Connecticut. For homes without tobacco combustion, the regional air monitoring site (Vinton, VA) appeared to provide a reasonable estimate of concentrations of PM2.5 and SO42- during summer months outside and inside homes within the region, even when a substantial number of the homes used air conditioning. Average indoor/outdoor ratios for PM2.5 and SO42- during the summer period were 1.03 +/- 0.71 and 0.74 +/- 0.53, respectively. The indoor/outdoor mean ratio for sulfate suggests that on average approximately 75% of the fine aerosol indoors during the summer is associated with outdoor sources. Kerosene heater use during the winter months, in the absence of tobacco combustion, results in substantial increases in indoor concentrations of PM2.5, SO42-, and possibly H+, as compared to homes without kerosene heaters. During their use, we estimated that kerosene heaters added, on average, approximately 40 microg/m3 of PM2.5 and 15 microg/m3 of SO42- to background residential levels of 18 and 2 microg/m3, respectively. Results from using sulfuric acid-doped Teflon (E.I. Du Pont de Nemours & Co., Wilmington, DE) filters in homes with kerosene heaters suggest that acid particle concentrations may be substantially higher than those measured because of acid neutralization by ammonia. During the summer and winter periods indoor concentrations of ammonia are an order of magnitude higher indoors than outdoors and appear to result in lower indoor acid particle concentrations. Nitrous acid levels are higher indoors than outdoors during both winter and summer and are substantially higher in homes with unvented combustion sources. ImagesFigure 1Figure 2Figure 3Figure 4Figure 5

DETERMINATION OF AEROSOL STRONG ACIDITY LOSSES DUE TO INTERACTIONS OF COLLECTED PARTICLES: RESULTS FROM LABORATORY AND FIELD STUDIES

Abstract Existing methods of measuring atmospheric aerosol strong acidity adequately prevent neutralization of fine-particle acidity by removing course alkaline particles and gaseous ammonia from air samples. However, these techniques do not consider particle interactions on the collection medium; therefore, they may still underestimate the actual aerosol acidity. Assessment of acid neutralization due to such interactions is made possible using annular denuder technology in conjuction with a newly designed filter pack. The amount of sulfate-related acidity neutralized by the collected ammonium nitrate (and possibly ammonium chloride and organic acid ammonium salts) is determined. Laboratory data suggest that large fractions of sulfate-related aerosol acidity are neutralized by ammonium nitrate particles during collection on filter media. Field data from the Harvard Acid Aerosol Health Effects Study also suggest that ammonium nitrate and possibly other ammonium salts, such as ammonium chloride, neutralize collected acid aerosols. For low-acid aerosol concentrations, the correction factor is significant; whereas, for high-acid concentrations, correction is negligible.

Evaluation of the gas collection of an annular denuder system under simulated atmospheric conditions

Abstract Laboratory studies evaluated the performance of a combined gas and particle sampling instrument. Results of these investigations indicated that the system had the ability to reliably sample atmospheric gases. The sampler consists of a glass inlet/impactor, two Na 2 CO 3 -coated annular denuders to collect gaseous SO 2 , HNO 3 and HNO 2 , a citric acid-coated annular denuder to trap NH 3 , and a filter pack to collect fine particles and artifact gases. The inlet walls may be extracted to measure the extent of gas deposition on the inlet surfaces. Inlet transmission efficiencies and denuder gas collection efficiencies indicated excellent performance under a wide range of simulated conditions. Laboratory experiments with SO 2 , HNO 3 and NH 3 at various concentrations and relative humidities (10−90%) indicated that the annular denuders achieve collection efficiencies near 100%. Tests to investigate the deposition of SO 2 , HNO 3 and NH 3 on the walls of the glass inlet showed a small loss ( 3 and NH 3 . No loss of SO 2 on inlet walls was detected. By extracting the inlet walls the deposited HNO 3 and NH 3 can be recovered.

Laboratory and field evaluation of measurement methods for one-hour exposures to O3, PM2.5, and CO.

ABSTRACT While researchers have linked acute (less than 12-hr) ambient O3, PM25, and CO concentrations to a variety of adverse health effects, few studies have characterized short-term exposures to these air pollutants, in part due to the lack of sensitive, accurate, and precise sampling technologies. In this paper, we present results from the laboratory and field evaluation of several new (or modified) samplers used in the “roll-around” system (RAS), which was developed to measure 1-hr O3, PM25, and CO exposures simultaneously. All the field evaluation data were collected during two sampling seasons: the summer of 1998 and the winter of 1999. To measure 1-hr O3 exposures, a new active O3 sampler was developed that uses two nitrite-coated filters to measure O3 concentrations. Laboratory chamber tests found that the active O3 sampler performed extremely well, with a collection efficiency of 0.96 that did not vary with temperature or relative humidity (RH). In field collocation comparisons with a reference UV photometric monitor, the active O3 sampler had an effective collection efficiency ranging between 0.92 and 0.96 and a precision for 1-hr measurements ranging between 4 and 6 parts per billion (ppb). The limits of detection (LOD) of this method were 9 ppb-hr for the chamber tests and ~16 ppb-hr for the field comparison tests. PM2.5 and CO concentrations were measured using modified continuous monitors—the DustTrak and the Langan, respectively. A size-selective inlet and a Nafion dryer were placed upstream of the DustTrak inlet to remove particles with aerodynamic diameters greater than 2.5 um and to dry particles prior to the measurements, respectively. During the field validation tests, the DustTrak consistently reported higher PM2.5 concentrations than those obtained by the collocated 12-hr PM2 5 PEM samples, by approximately a factor of 2. After the DustTrak response was corrected (correction factor of 2.07 in the summer and 2.02 in the winter), measurements obtained using these methods agreed well with R2 values of 0.87 in the summer and 0.81 in the winter. The results showed that the DustTrak can be used along with integrated measurements to measure the temporal and spatial variation in PM2 5 exposures. Finally, during the field validation tests, CO concentrations measured using the Langan were strongly correlated with those obtained using the reference method when the CO levels were above the LOD of the instrument [~1 part per million (ppm)].

Design of a Glass Impactor for an Annular Denuder / Filter Pack System

A glass impactor for an annular denuder/filter pack system was developed, to further the application of denuder technology in sampling atmospheric gases and particles. The glass impactor consists of an entrance section containing the inlet tube, the acceleration jet, and the impaction plate, which is mounted at the entrance to the annular denuder. The impaction plate is a removable porous glass disk which can be impregnated with mineral oil to minimize bounce-off of the collected particles during sampling. Calibration tests showed that the impactor has a 50% aerodynamic particle cutoff size of 2.1 μm, at a flow of 10 L min−1. Particle loss experiments were conducted. Total losses on surfaces inside the impactor, annular denuder, and filter pack, determined for particle sizes ranging between 1.50 and 2.77 μm, were lower than 3%. Co-located air sampling was conducted using the glass impactor and the Harvard impactor. Mass concentrations determined using the Harvard impactor were about 10% higher than for th...

DEVELOPMENT AND VALIDATION OF A HIGH-VOLUME, LOW-CUTOFF INERTIAL IMPACTOR

A low-cutoff, high-volume conventional impactor has been designed. This sampler uses a slit-shaped acceleration jet and operates at 1100 L/min. The impaction substrate is polyurethane foam (PUF). The impactor collection efficiency was characterized using polydisperse particles, and the 50% size cutoff point was 0.12 ¡m. Losses within the sampler were also characterized and were less than 10%. The use of polyurethane foam (PUF) as a substrate has the following advantages: (I) PUF has a very high particle collection efficiency over a large range of particle sizes, even under conditions of heavy particle loading, as compared to other impaction substrates, such as flat plates and less porous membranes, which typically are subject to significant bounce-off and reentrainment; (2) no oil or grease coating is required, so potential interferences of impurities within such coatings are avoided when chemical, biological, and toxicological tests are performed on the collected particles; (3) PUF itself is chemically inert, minimizing interference with any of these tests; (4) because of the high flow rate of 1100 L/min, a large amount of particles can be collected in a short period of time on a relatively small surface of substrate, facilitating recovery of the collected particles for the different tests; and (5) a large amount of particles can be collected on a relatively small collection surface and easily extracted with small amounts of water or organic solvents. This method will be suitable for the collection of large amounts for toxicological studies and analysis of organic aerosols, which is not possible with other high-volume samplers that utilize large filtration surfaces.

Aged particles derived from emissions of coal-fired power plants: The TERESA field results

The Toxicological Evaluation of Realistic Emissions Source Aerosols (TERESA) study was carried out at three US coal-fired power plants to investigate the potential toxicological effects of primary and photochemically aged (secondary) particles using in situ stack emissions. The exposure system designed successfully simulated chemical reactions that power plant emissions undergo in a plume during transport from the stack to receptor areas (e.g., urban areas). Test atmospheres developed for toxicological experiments included scenarios to simulate a sequence of atmospheric reactions that can occur in a plume: (1) primary emissions only; (2) H2SO4 aerosol from oxidation of SO2; (3) H2SO4 aerosol neutralized by gas-phase NH3; (4) neutralized H2SO4 with secondary organic aerosol (SOA) formed by the reaction of α-pinene with O3; and (5) three control scenarios excluding primary particles. The aged particle mass concentrations varied significantly from 43.8 to 257.1 µg/m3 with respect to scenario and power plant. The highest was found when oxidized aerosols were neutralized by gas-phase NH3 with added SOA. The mass concentration depended primarily on the ratio of SO2 to NOx (particularly NO) emissions, which was determined mainly by coal composition and emissions controls. Particulate sulfate (H2SO4 + neutralized sulfate) and organic carbon (OC) were major components of the aged particles with added SOA, whereas trace elements were present at very low concentrations. Physical and chemical properties of aged particles appear to be influenced by coal type, emissions controls and the particular atmospheric scenarios employed.