Final Report: Characterization of the Chemical Composition of Atmospheric Ultrafine Particles

EPA Grant Number: R827354C001
Subproject: this is subproject number 001 , established and managed by the Center Director under grant R827354
(EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).

Center: Airborne PM - Rochester PM Center
Center Director: Oberdörster, Günter
Title: Characterization of the Chemical Composition of Atmospheric Ultrafine Particles
Investigators: Cass, Glen , Dillner, Ann , Hopke, Philip K. , Prather, Kimberly A.
Institution: Georgia Institute of Technology , Arizona State University - Main Campus , Clarkson University , University of California - Riverside
EPA Project Officer: Chung, Serena
Project Period: June 1, 1999 through May 31, 2005 (Extended to May 31, 2006)
RFA: Airborne Particulate Matter (PM) Centers (1999) RFA Text |  Recipients Lists
Research Category: Air Quality and Air Toxics , Particulate Matter , Air

Objective:

The objective of this research project is to identify the chemical composition of atmospheric ultrafine particle samples that will be collected in field experiments in Houston, TX, seven cities in Southern CA, and Riverside, CA. Three research groups, at the Georgia Institute of Technology (GIT), Arizona State University (ASU), and the University of California–San Diego (UCSD), are collaborating on this research project.

Summary/Accomplishments (Outputs/Outcomes):

In the early stage of this project, the state of knowledge of the composition of ultrafine particles was summarized by Cass, et al. (2000). The Cass/Dillner group collected ultrafine particle samples in field experiments in a south central U.S. city (Houston, TX) and in a west coast city (Riverside, CA). A cluster analysis was applied by Dillner, et al., (2005) using data from two sites in Houston, TX; one site surrounded by refineries, chemical plants, and vehicular and commercial shipping traffic, and the other site, 25 miles inland surrounded by residences, light industrial facilities, and vehicular traffic. Twenty-four hour size-segregated (0.056 μm < Dp (particle diameter) <1.8 μm) particulate matter samples were collected during five days in August 2000. Inductively coupled plasma mass spectrometry (ICPMS) was used to quantify 32 elements with concentrations as low as a few picograms per cubic meter. Concentrations of particulate matter mass, sulfate and organic carbon at the two sites were often not significantly different from each other and had smooth unimodal size distributions indicating the regional nature of these species. Element concentrations varied widely across events and sites and often showed sharp peaks at particle diameters between 0.1 and 0.3 μm and in the ultrafine mode (Dp <0.1 μm) that suggested the sources of these elements were local, high temperature processes. Elements were clustered to provide normalized size distributions of all elements and to yield groups of elements with similar size distributions that were attributed to sources such as automobile catalysts, fluid catalytic cracking unit catalysts, fuel oil burning, a coal-fired power plant, and high-temperature metal working. The clustered elements were generally attributed to different sources at the two sites during each sampling day indicating the diversity of local sources that impact heavy metals concentrations in the areas around the sampling sites.

Su, et al., (2004) described the development of an improved aerosol time of flight mass spectrometry (ATOFMS) instrument to measure the chemical composition of single atmospheric particles smaller than 100 nm in particle diameter. An ultrafine particle aerosol time of flight mass spectrometry instrument has been constructed incorporating an aerodynamic lens system that allows transmission of ultrafine particles into the instrument. An effective method for detecting ultrafine particles in the systems has been developed and used in a number of ambient aerosol characterization studies including studies supported by the Center and many others. Thus, the development effort supported under this Core has lead to a significant advance in ultrafine particle characterization that has broadened our understanding of their chemical composition.

To further support the field studies, Spencer and Prather (2006) used laboratory generated ultrafine particles to demonstrate the ability to quantify the amount of organic carbon (OC) on elemental carbon (EC) particles. They coated generated EC particles and developed a calibration curve that permitted the quantification of the amount of OC on EC particles. This resulting calibration curve was used to calculate the OC/EC mass fraction for particles in lab studies; field studies in Boston, San Diego, and Atlanta; and in two source studies (gasoline and diesel vehicles). In addition, this calibration curve was used to show that 30% of the additional OC coating observed in particles produced by an ultrafine concentrator were being added to ultrafine particles in the concentrator (Su, et al., 2006). This change was attributed to additional gas-particle partitioning in the humidified growth region.

A study was conducted in Riverside, CA during the summer and fall of 2005. This was a large field study focused on PM2.5 organic aerosols. In addition to standard gas, aerosol, and PM measurements, as part of this project, ultrafine particles were measured using a UF-ATOFMS for 3 weeks during both of these studies. In addition to standard ambient sampling and characterization, ambient particles were size selected using a Scanning Mobility Particle Sizer (SMPS). The aerodynamic sizes of these particles were measured in the ATOFMS. These two sizes could be used to determine the density and shape of ambient EC particles. It was determined that most of the particles in the summer had different densities on different days and times of the day. These densities were strongly dependent on the atmospheric water content. The higher the water content, the lower the particle density. This result suggested the Riverside summer aerosol was highly processed, allowing significant uptake of water (Spencer and Prather, 2007). Spencer, et al. (2006) reported the development of a procedure to make diesel lubricating oil particles and showed how similar their ATOFMS spectra were to ambient particles from diesel vehicles.

Beginning at the end of November 2001, the number concentrations of ultrafine particles have been measured at the NYS Department of Environmental Conservation (DEC) monitoring site on the central fire station in downtown Rochester, NY. Particle size distributions are being measured using an SMPS comprised of a differential mobility analyzer (DMA) and a condensation particle counter (CPC). In the diameter range of 10 to 500 nm, ambient particles are classified by a DMA (TSI 3071) and counted with a CPC (TSI 3010) every five minutes. This work was originally supported by the New York State Energy Research and Development Authority, but at the end of that support, the work was continued with Center support. We have 1.5 years of data providing information on the number distributions of particles between 10 and 500 nm. In addition, the DEC site monitors SO2, CO, PM2.5, and meteorological variables. The results of this monitoring have been reported by Jeong, et al. (2004a; 2006). More than 70% of measured total number concentration was associated with ultrafine particles (UFP, 0.011-0.050 µm). Morning nucleation events typically peaking UFP number concentrations at around 8:00 were apparent in winter months with CO increases. These particles appear to be formed following direct emissions from motor vehicles during morning rush hour. There were also often observed increases in this smaller sized range particles in the late afternoon during the afternoon rush hour particularly in winter when the mixing heights remain lower than in summer. Strong afternoon nucleation events (> 30,000 cm-3) peaking at around 13:00 were more likely to occur in spring and summer months. During the prominent nucleation events, peaks of SO2 were strongly associated with the number concentrations of UFP, whereas there were no significant correlations between these events and PM2.5 and CO. Increased SO2 concentrations were observed when the wind direction was northwesterly where three SO2 sources were located. It is hypothesized that UFP formed during the events are sulfuric acid and water from the oxidation of SO2. There was also a more limited number of nucleation events followed by particle growth up to approximately 0.1 µm over periods of up to 18 hours. The nucleation and growth events tended to be common in spring months especially in April.

As part of the Core’s effort to characterize the nature of PM2.5, measurements of particle composition were made in Rochester, Philadelphia, and New York City that have been reported by Jeong, et al. (2004b,c) and Venkatachari, et al. (2006a,b). A major contribution of this Core has been the initiation of study of particle-bound reactive oxygen species (ROS). There is currently very limited information available on particle-bound ROS and thus, measurements in Rubidoux, CA (Venkatachari, et al., 2005) and New York City (Venkatachari, et al., 2007) suggest that there can be significant concentrations of oxidant on fine particle surfaces. Studies of the effects of the particle-bound ROS are planned for the future at the University of Rochester.

References:

Cass GR, et al. The chemical composition of atmospheric ultrafine particles. The Philosophical Transactions of the Royal Society (Series A) 2000;358:2581-2592.

Dillner AM, Schauer JJ, Christensen WF, Cass GR. A quantitative method for clustering size distributions of elements. Atmospheric Environment 2005;39:1525–1537.

JeongC-H, Hopke PK, Chalupa D, Utell M. Characteristics of nucleation and growth events of ultrafine particles measured in Rochester, NY. Environmental Science & Technology 2004a;38(No.7):1933-1940.

Jeong C-H, Lee D-W, Kim E, Hopke PK. Measurement of real-time PM2.5 mass, sulfate, and carbonaceous aerosols at the multiple monitoring sites. Atmospheric Environment 2004b;38:5247-5256.

Jeong C-H, Hopke PK, Kim E, Lee D-W. The comparison between thermal-optical transmittance elemental carbon and Aethalometer black carbon measured at the multiple monitoring sites. Atmospheric Environment 2004c;38:5193-5204.

Jeong C-H, Evans GJ, Hopke PK, Chalupa D, Utell MJ. Influence of atmospheric dispersion and new particle formation events on ambient particle number concentration in Rochester, United States, and Toronto, Canada. Journal of the Air & Waste Management Association 2006;56:431-443.

Spencer MT, Prather KA. Using ATOFMS to determine OC/EC mass fractions in particles. Aerosol Science and Technology 2006;40:585-594.

Spencer M, Prather K. Measurements of the density of atmospheric aerosols. Environmental Science & Technology 2007;41:1303-1309.

Spencer MT, Prather KA, Shields LG. Chemical analysis of used and new petroleum-based lubricants using ATOFMS. Atmospheric Environment 2006;40:5224-5235.

Su YX, Sipin MF, Furutani H, Prather KA. Development and characterization of an ATOFMS with increased detection efficiency. Analytical Chemistry 2004;76(3):712-719.

Su YX, Sipin MF, Spencer MT, Qin X, Moffet RC, Shields LG, Prather KA, Venkatachari P, Jeong CH, Kim E, Hopke PK, Gelein RM, Utell MJ, Oberdorster G, Berntsen J, Devlin RB, Chen LC. Real-time characterization of the composition of individual particles emitted from ultrafine particle concentrators. Aerosol Science and Technology 2006;40(No. 6):437-455.

Venkatachari P, Hopke PK, Grover BD, Eatough DJ. Measurement of particle-bound reactive oxygen species in rubidoux aerosols. Journal of Atmospheric Chemistry 2005;50:49-58.

Venkatachari P, Zhou L, Hopke PK, Schwab JJ, Demerjian KL, Weimer S, Hogrefe O, Felton D, Rattigan O. An intercomparison of measurement methods for carbonaceous aerosol in the ambient air in New York City. Aerosol Science and Technology 2006a;40:788-795.

Venkatachari P, Zhou L, Hopke PK, Felton D, Rattigan OV, Schwab JJ, Demerjian KL. Spatial and temporal variability of black carbon in New York City. Journal of Geophysical Research 2006b;111:D10S05, doi:10.1029/2005JD006314.

Venkatachari P, Hopke PK, Brune WH, Ren X, Lesher R, Mao J, Mitchell M. Characterization of wintertime reactive oxygen species concentrations in flushing, New York. Aerosol Science and Technology 2007;41:97-111.

Technical Report:

Full Final Technical Report (PDF, 5pp., 22.3KB, about PDF)


Journal Articles on this Report : 29 Displayed | Download in RIS Format

Other subproject views: All 30 publications 30 publications in selected types All 29 journal articles
Other center views: All 104 publications 98 publications in selected types All 90 journal articles
Type Citation Sub Project Document Sources
Journal Article Cass GR, Hughes LA, Bhave P, Kleeman MJ, Allen JO, Salmon LG. The chemical composition of atmospheric ultrafine particles. Philosophical Transactions of the Royal Society of London Series A-Mathematical Physical & Engineering Sciences 2000;358(1775):2581-2592. R827354 (2004)
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  • Journal Article Dillner AM, Schauer JJ, Christensen WF, Cass GR. A quantitative method for clustering size distributions of elements. Atmospheric Environment 2005;39(8):1525-1537. R827354 (2004)
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  • Journal Article Elder A, Couderc J-P, Gelein R, Eberly S, Cox C, Xia X, Zareba W, Hopke P, Watts W, Kittelson D, Frampton M, Utell M, Oberdorster G. Effects of on-road highway aerosol exposures on autonomic responses in aged, spontaneously hypertensive rats. Inhalation Toxicology 2007;19(1):1-12. R827354 (Final)
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  • Journal Article Hopke PK, Ito K, Mar T, Christiansen WF, Eatough DJ, Henry RC, Kim E, Laden F, Lall R, Larson TV, Liu H, Neas L, Pinto J, Stolzel M, Suh H, Paatero P, Thurston GD. PM source apportionment and health effects:1. Intercomparison of source apportionment results. Journal of Exposure Science & Environmental Epidemiology 2006;16(3):275-286. R827354 (Final)
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  • Journal Article Ito K, Christensen WF, Eatough DJ, Henry RC, Kim E, Laden F, Lall R, Larson TV, Neas L, Hopke PK, Thurston GD. PM source apportionment and health effects: 2. An investigation of intermethod variability in associations between source-apportioned fine particle mass and daily mortality in Washington, DC. Journal of Exposure Science & Environmental Epidemiology 2006;16(4):300-310. R827354 (Final)
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  • Journal Article Jeong C-H, Hopke PK, Chalupa D, Utell M. Characteristics of nucleation and growth events of ultrafine particles measured in Rochester, NY. Environmental Science & Technology 2004;38(7):1933-1940. R827354 (Final)
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  • Journal Article Jeong C-H, Lee D-W, Kim E, Hopke PK. Measurement of real-time PM2.5 mass, sulfate, and carbonaceous aerosols at the multiple monitoring sites. Atmospheric Environment 2004;38(31):5247-5256. R827354 (Final)
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  • Journal Article Jeong C-H, Hopke PK, Kim E, Lee D-W. The comparison between thermal-optical transmittance elemental carbon and Aethalometer black carbon measured at multiple monitoring sites. Atmospheric Environment 2004;38(31):5193-5204. R827354 (Final)
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  • Journal Article Jeong C-H, Evans GJ, Hopke PK, Chalupa D, Utell MJ. Influence of atmospheric dispersion and new particle formation events on ambient particle number concentration in Rochester, United States, and Toronto, Canada. Journal of the Air & Waste Management Association 2006;56(4):431-443. R827354 (Final)
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  • Journal Article Kim E, Larson TV, Hopke PK, Slaughter C, Sheppard LE, Claiborn C. Source identification of PM2.5 in an arid Northwest U.S. city by positive matrix factorization. Atmospheric Research 2003;66(4):291-305. R827354 (Final)
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  • Journal Article Kim E, Hopke PK, Larson TV, Maykut NN, Lewtas J. Factor analysis of Seattle fine particles. Aerosol Science and Technology 2004;38(7):724-738. R827354 (Final)
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  • Journal Article Kim E, Hopke PK, Larson TV, Covert DS. Analysis of ambient particle size distributions using Unmix and positive matrix factorization. Environmental Science & Technology 2004;38(1):202-209. R827354 (Final)
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  • Journal Article Kittelson DB, Watts WF, Johnson JP, Remerowki ML, Ische EE, Oberdorster G, Gelein RM, Elder A, Hopke PK, Kim E, Zhao W, Zhou L, Jeong C-H. On-road exposure to highway aerosols. 1. Aerosol and gas measurements. Inhalation Toxicology 2004;16(Suppl 1):31-39. R827354 (Final)
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  • Journal Article Mar TF, Ito K, Koenig JQ, Larson TV, Eatough DJ, Henry RC, Kim E, Laden F, Lall R, Neas L, Stolzel M, Paatero P, Hopke PK, Thurston GD. PM source apportionment and health effects. 3. Investigation of inter-method variations in associations between estimated source contributions of PM2.5 and daily mortality in Phoenix, AZ. Journal of Exposure Science & Environmental Epidemiology 2006;16(4):311-320. R827354 (Final)
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  • Journal Article Moffet RC, Shields LG, Berntsen J, Devlin RB, Prather KA. Characterization of an ambient coarse particle concentrator used for human exposure studies: aerosol size distributions, chemical composition, and concentration enrichment. Aerosol Science and Technology 2004;38(11):1123-1137. R827354 (Final)
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  • Journal Article Ogulei D, Hopke PK, Chalupa DC, Utell MJ. Modeling source contributions to submicron particle number concentrations measured in Rochester, New York. Aerosol Science and Technology 2007;41(2):179-201. R827354 (Final)
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  • Journal Article Spencer MT, Prather KA. Using ATOFMS to determine OC/EC mass fractions in particles. Aerosol Science and Technology 2006;40(8):585-594. R827354 (Final)
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  • Journal Article Spencer MT, Shields LG, Sodeman DA, Toner SM, Prather KA. Comparison of oil and fuel particle chemical signatures with particle emissions from heavy and light duty vehicles. Atmospheric Environment 2006;40(27):5224-5235. R827354 (Final)
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  • Journal Article Su Y, Sipin MF, Furutani H, Prather KA. Development and characterization of an aerosol time-of-flight mass spectrometer with increased detection efficiency. Analytical Chemistry 2004;76(3):712-719. R827354 (Final)
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  • Journal Article Su Y, Sipin MF, Prather KA, Gelein RM, Lunts A, Oberdorster G. ATOFMS characterization of individual model aerosol particles used for exposure studies. Aerosol Science and Technology 2005;39(5):400-407. R827354 (Final)
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  • Journal Article Su Y, Sipin MF, Spencer MT, Qin X, Moffet RC, Shields LG, Prather KA, Venkatachari P, Jeong C-H, Kim E, Hopke PK, Gelein RM, Utell MJ, Oberdorster G, Berntsen J, Devlin RB, Chen LC. Real-time characterization of the composition of individual particles emitted from ultrafine particle concentrators. Aerosol Science and Technology 2006;40(6):437-455. R827354 (Final)
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  • Journal Article Thurston GD, Ito K, Mar T, Christensen WF, Eatough DJ, Henry RC, Kim E, Laden F, Lall R, Larson TV, Liu H, Neas L, Pinto J, Stolzel M, Suh H, Hopke PK. Workgroup report: Workshop on source apportionment of particulate matter health effects—intercomparison of results and implications. Environmental Health Perspectives 2005;113(12):1768-1774. R827354 (Final)
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  • Journal Article Toner SM, Shields LG, Sodeman DA, Prather KA. Using mass spectral source signatures to apportion exhaust particles from gasoline and diesel powered vehicles in a freeway study using UF-ATOFMS. Atmospheric Environment 2008;42(3):568-581. R827354 (Final)
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  • Journal Article Venkatachari P, Hopke PK, Grover BD, Eatough DJ. Measurement of particle-bound reactive oxygen species in rubidoux aerosols. Journal of Atmospheric Chemistry 2005;50(1):49-58. R827354 (Final)
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  • Journal Article Venkatachari P, Zhou L, Hopke PK, Felton D, Rattigan OV, Schwab JJ, Demerjian KL. Spatial and temporal variability of black carbon in New York City. Journal of Geophysical Research 2006;111(D10):D10S05 (9 pp.). R827354 (Final)
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  • Journal Article Venkatachari P, Zhou L, Hopke PK, Schwab JJ, Demerjian KL, Weimer S, Hogrefe O, Felton D, Rattigan O. An intercomparison of measurement methods for carbonaceous aerosol in the ambient air in New York City. Aerosol Science and Technology 2006;40(10):788-795. R827354 (Final)
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    R832415 (2011)
    R832415 (Final)
  • Full-text: Taylor & Francis-Full Text HTML
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  • Abstract: Taylor & Francis-Abstract
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  • Other: Taylor & Francis-Full Text PDF
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  • Journal Article Zhao W, Hopke PK, Qin X, Prather KA. Predicting bulk ambient aerosol compositions from ATOFMS data with ART-2a and multivariate analysis. Analytica Chimica Acta 2005;549(1-2):179-187. R827354 (Final)
    R827354C001 (Final)
    R831083 (Final)
    R832415 (2010)
    R832415 (2011)
    R832415 (Final)
  • Full-text: ScienceDirect-Full Text HTML
    Exit
  • Abstract: ScienceDirect-Abstract
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  • Other: ScienceDirect-Full Text PDF
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  • Journal Article Zhou L, Kim E, Hopke PK, Stanier C, Pandis SN. Mining airborne particulate size distribution data by positive matrix factorization. Journal of Geophysical Research 2005;110(D7):D07S19 (15 pp.). R827354 (Final)
    R827354C001 (Final)
    R832415 (2010)
    R832415 (2011)
    R832415 (Final)
  • Full-text: Wiley Online-Full Text HTML
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  • Abstract: Wiley Online-Abstract
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  • Other: University of Iowa-Full Text PDF
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  • Journal Article Zhou L, Hopke PK, Venkatachari P. Cluster analysis of single particle mass spectra at Flushing, NY. Analytica Chimica Acta 2006;555(1):47-56. R827354 (Final)
    R827354C001 (Final)
    R832415 (2010)
    R832415 (2011)
    R832415 (Final)
  • Full-text: ScienceDirect-Full Text HTML
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  • Abstract: ScienceDirect-Abstract
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  • Other: ScienceDirect-Full Text PDF
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  • Supplemental Keywords:

    RFA, Health, Scientific Discipline, Air, Geographic Area, particulate matter, Environmental Chemistry, Health Risk Assessment, Epidemiology, State, Risk Assessments, Biochemistry, ambient air quality, particle size, particulates, sensitive populations, cardiopulmonary responses, fine particles, human health effects, morbidity, ambient air monitoring, chemical characteristics, pulmonary disease, susceptible populations, epidemelogy, environmental health effects, particle exposure, nano differential mobility analyzer, human exposure, particulate exposure, chemical kinetics, Texas (TX), PM, mortality, urban environment, aerosols, ultrafine particles, chemical speciation sampling

    Relevant Websites:

    Full Final Technical Report (PDF, 5pp., 22.3KB, about PDF)
    http://www2.envmed.rochester.edu/envmed/PMC/indexPMC.html Exit

    Progress and Final Reports:

    Original Abstract
  • 1999 Progress Report
  • 2000 Progress Report
  • 2001 Progress Report
  • 2002 Progress Report
  • 2003 Progress Report
  • 2004 Progress Report

  • Main Center Abstract and Reports:

    R827354    Airborne PM - Rochester PM Center

    Subprojects under this Center: (EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).
    R827354C001 Characterization of the Chemical Composition of Atmospheric Ultrafine Particles
    R827354C002 Inflammatory Responses and Cardiovascular Risk Factors in Susceptible Populations
    R827354C003 Clinical Studies of Ultrafine Particle Exposure in Susceptible Human Subjects
    R827354C004 Animal Models: Dosimetry, and Pulmonary and Cardiovascular Events
    R827354C005 Ultrafine Particle Cell Interactions: Molecular Mechanisms Leading to Altered Gene Expression
    R827354C006 Development of an Electrodynamic Quadrupole Aerosol Concentrator
    R827354C007 Kinetics of Clearance and Relocation of Insoluble Ultrafine Iridium Particles From the Rat Lung Epithelium to Extrapulmonary Organs and Tissues (Pilot Project)
    R827354C008 Ultrafine Oil Aerosol Generation for Inhalation Studies