Final Report: Development and Deployment of an Instrumentation Suite for Comprehensive Air Quality Characterization Including Aerosol ROS

EPA Grant Number: R834799C001
Subproject: this is subproject number 001 , established and managed by the Center Director under grant R834799
(EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).

Center: The Southeastern Center for Air Pollution and Epidemiology: Multiscale Measurements and Modeling of Mixtures
Center Director: Tolbert, Paige
Title: Development and Deployment of an Instrumentation Suite for Comprehensive Air Quality Characterization Including Aerosol ROS
Investigators: Weber, Rodney J. , Bergin, Michael , Mulholland, James , Nenes, Athanasios , Sarnat, Stefanie Ebelt , Sarnat, Jeremy , Strickland, Matthew J
Institution: Georgia Institute of Technology , Duke University , Emory University , University of Nevada - Reno
EPA Project Officer: Chung, Serena
Project Period: January 1, 2011 through December 31, 2016
RFA: Clean Air Research Centers (2009) RFA Text |  Recipients Lists
Research Category: Health Effects , Air

Objective:

To provide a chemically comprehensive data set on ambient particle composition at various sites relative to roadway emissions that will be used by other Southeast Center for Air Pollution & Epidemiology (SCAPE) projects. As a part of this effort, our goal is to develop new instruments and analytical methods to quantify concentrations of particle-bound reactive oxygen species (ROS) and associated aerosol components. These techniques were deployed during SCAPE and data sets have been generated for investigating ROS sources, atmospheric processing, and health impacts.

Summary/Accomplishments (Outputs/Outcomes):

During this reporting period, work has focused on completing experiments, data analyses, and publishing papers. The following experiments are underway:

MOUDI Size Distribution Measurements of DTT and AA: Multi-orifice impactors (MOUDIs) were deployed simultaneously at the roadside and near-road side (Georgia Tech) sites. A suite of analyses have been done on the samples, including water soluble dithiothreitol (DTT), total DTT, ascorbic acid (AA), ions (both anions and cations), OC, EC, and both water soluble metals and total metals. The data provide insight on sources and process that affect AA and DTT, complementary to the source apportionment and other methods we have used in the past. The data also provide unique insight on deposition of DTT and AA in a human respiratory system.

Analysis of DTT activity of Isoprene Secondary Organic Aerosol (SOA): Published data from other investigators suggest that isoprene SOA is as toxic as diesel aerosol processed in a smog chamber (Kramer, et al., Atmospheric Environment 2015). These results contrast to our SCAPE findings that show isoprene OA is one of the least DTT active components of the aerosol. To explore this, we collaborated with the Caltech Seinfeld group on running a comprehensive series of isoprene chamber SOA experiments, and analyzed the DTT activity on the filter samples they provided. These results are still incomplete, but our preliminary results agree with ambient data; isoprene has generally low DTT activity. The analysis shows that what really is happening is that the DTT activity of diesel emissions aged in a chamber are much lower than our ambient SCAPE data. Thus it is not that isoprene is DTT active, it is that chambers cannot chemically age the diesel emissions such that the toxicity reaches levels seen in our ambient studies.

Development of method for Total DTT measurement: SCAPE has focused on water soluble DTT components; however, there is reported research showing that DTT activity can also be associated with insoluble particles. We developed a method to measure the insoluble plus soluble DTT active components of PM2.5 and are testing it by comparing filter samples collected simultaneously at a central Atlanta site (GIT) and one or two roadside sites where insoluble species are expected to be higher due to association with soot and/or road dust. The two roadside sites have differing levels of diesel traffic. The work is in progress, but expected to be finished by the end of summer 2016.

Continued work on an Online ROS system: Although the filter-based system has provided major new insights, it is recognized that online measurements of ROS by acellular assays, such as DTT, could provide substantially greater insights into sources, atmospheric processing and health impacts of aerosols. An online system provides much larger data sets, allows better integration with state-of-the art online aerosol chemical speciation instrumentation, provides a better assessment of variability in ROS and what drives it, and provides an assessment of possible artifacts associated with filter-based methods. In the past year, progress has been made on developing the method. Methods developed in the last 2 years with a particle-into-liquid sampler (PILS) coupled to the DTT analytical system have proven to be unstable. We now are switching to a Mist Chamber-type system to collect the aerosol. Tests will be undertaken to apply the system for both water soluble and possibly total DTT.

Ongoing work on the Stability of ROS on Filters: Linking ROS to health endpoints through epidemiological analysis requires knowledge of ROS over an extended period of time. Since our approach is a retrospective analysis, ROS (DTT) data from the JST site was estimated based on a source apportionment analyses. To verify predicted ROS and assess uncertainty, we proposed to measure ROS on archived filters. This approach is based on the assumption that DTT is stable on frozen filters for extended time periods. To assess this, we performed experiments on filters collected by SEARCH at JST during the period when ROS was measured at JST as part of this project. These filters have been stored for over two years. We also collected filters roughly 1.5 years ago specifically for this experiment. We continue to test these filters to develop an increasingly long time-trend on stability.


Journal Articles on this Report : 17 Displayed | Download in RIS Format

Other subproject views: All 62 publications 17 publications in selected types All 17 journal articles
Other center views: All 302 publications 104 publications in selected types All 100 journal articles
Type Citation Sub Project Document Sources
Journal Article Bates JT, Weber RJ, Abrams J, Verma V, Fang T, Klein M, Strickland MJ, Sarnat SE, Chang HH, Mulholland JA, Tolbert PE, Russell AG. Reactive oxygen species generation linked to sources of atmospheric particulate matter and cardiorespiratory effects. Environmental Science & Technology 2015;49(22):13605-13612. R834799 (2015)
R834799 (2016)
R834799 (Final)
R834799C001 (Final)
R834799C003 (Final)
R834799C004 (2015)
R834799C004 (Final)
  • Abstract from PubMed
  • Full-text: ES&T-Full Text HTML
    Exit
  • Abstract: ES&T-Abstract
    Exit
  • Other: ES&T-Full Text PDF
    Exit
  • Journal Article Budisulistiorini SH, Canagaratna MR, Croteau PL, Baumann K, Edgerton ES, Kollman MS, Ng NL, Verma V, Shaw SL, Knipping EM, Worsnop DR, Jayne JT, Weber RJ, Surratt JD. Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in downtown Atlanta, Georgia. Atmospheric Measurement Techniques 2014;7(7):1929-1941. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text: AMT-Full Text PDF
    Exit
  • Abstract: AMT-Abstract
    Exit
  • Other: Harvard University-Abstract
    Exit
  • Journal Article Fang T, Verma V, Guo H, King LE, Edgerton ES, Weber RJ. A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE). Atmospheric Measurement Techniques 2015;8(1):471-482. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text: AMT-Full Text PDF
    Exit
  • Abstract: AMT-Abstract
    Exit
  • Other: Harvard University-Abstract
    Exit
  • Journal Article Fang T, Guo H, Verma V, Peltier RE, Weber RJ. PM2.5 water-soluble elements in the southeastern United States: automated analytical method development, spatiotemporal distributions, source apportionment, and implications for heath studies. Atmospheric Chemistry and Physics 2015;15(20):11667-11682. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Other: ResearchGate-Abstract & Full Text PDF
    Exit
  • Journal Article Fang T, Verma V, Bates JT, Abrams J, Klein M, Strickland MJ, Sarnat SE, Chang HH, Mulholland JA, Tolbert PE, Russell AG, Weber RJ. Oxidative potential of ambient water-soluble PM2.5 in the southeastern United States: contrasts in sources and health associations between ascorbic acid (AA) and dithiothreitol (DTT) assays. Atmospheric Chemistry and Physics 2016;16(6):3865-3879. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (Final)
    R834799C003 (Final)
    R834799C004 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Other: ResearchGate-Abstract & Full Text PDF
    Exit
  • Journal Article Guo H, Xu L, Bougiatioti A, Cerully KM, Capps SL, Hite Jr. JR, Carlton AG, Lee S-H, Bergin MH, Ng NL, Nenes A, Weber RJ. Fine-particle water and pH in the southeastern United States. Atmospheric Chemistry and Physics 2015;15(9):5211-5228. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
    R835041 (2015)
    R835041 (Final)
    R835410 (2013)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Other: ResearchGate-Abstract & Full Text PDF
    Exit
  • Journal Article King LE, Weber RJ. Development and testing of an online method to measure ambient fine particulate Reactive Oxygen Species (ROS) based on the 2’,7’-dichlorofluorescin (DCFH) assay. Atmospheric Measurement Techniques 2013;6(7):1647-1658. R834799 (2013)
    R834799 (2014)
    R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2013)
    R834799C001 (2014)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text: Atmospheric Measurement Techniques-Full Text PDF
    Exit
  • Abstract: Atmospheric Measurement Techniques-Abstract
    Exit
  • Journal Article Liu J, Bergin M, Guo H, King L, Kotra N, Edgerton E, Weber RJ. Size-resolved measurements of brown carbon in water and methanol extracts and estimates of their contribution to ambient fine-particle light absorption. Atmospheric Chemistry and Physics 2013;13(24):12389-12404. R834799 (2014)
    R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2013)
    R834799C001 (2014)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text: Atmospheric Chemistry and Physics-Full Text PDF
    Exit
  • Abstract: Atmospheric Chemistry and Physics-Abstract
    Exit
  • Other: ResearchGate-Full Text PDF
    Exit
  • Journal Article Liu J, Scheuer E, Dibb J, Ziemba LD, Thornhill KL, Anderson BE, Wisthaler A, Mikoviny T, Devi JJ, Bergin M, Weber RJ. Brown carbon in the continental troposphere. Geophysical Research Letters 2014;41(6):2191-2195. R834799 (2014)
    R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2014)
    R834799C001 (2015)
    R834799C001 (Final)
    R835039 (Final)
  • Full-text: Wiley-Full Text PDF
    Exit
  • Abstract: Wiley-Abstract & Full Text HTML
    Exit
  • Other: ResearchGate-Full Text PDF
    Exit
  • Journal Article Sarnat SE, Chang HH, Weber RJ. Ambient PM2.5 and health: does PM2.5 oxidative potential play a role? American Journal of Respiratory and Critical Care Medicine 2016;194(5):530-531. R834799 (2016)
    R834799 (Final)
    R834799C001 (Final)
    R834799C004 (Final)
  • Abstract from PubMed
  • Abstract: AJRCCM-PDF Preview
    Exit
  • Journal Article Verma V, Rico-Martinez R, Kotra N, King L, Liu J, Snell TW, Weber RJ. Contribution of water-soluble and insoluble components and their hydrophobic/hydrophilic subfractions to the reactive oxygen species-generating potential of fine ambient aerosols. Environmental Science & Technology 2012;46(20):11384-11392. R834799 (2012)
    R834799 (2013)
    R834799 (2014)
    R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2012)
    R834799C001 (2013)
    R834799C001 (2014)
    R834799C001 (2015)
    R834799C001 (Final)
  • Abstract from PubMed
  • Full-text: ES&T-Full Text PDF
    Exit
  • Abstract: ES&T-Abstract
    Exit
  • Other: ResearchGate-Full Text PDF
    Exit
  • Journal Article Verma V, Rico-Martinez R, Kotra N, Rennolds C, Liu J, Snell TW, Weber RJ. Estimating the toxicity of ambient fine aerosols using freshwater rotifer Brachionus calyciflorus (Rotifera: Monogononta). Environmental Pollution 2013;182:379-384. R834799 (2014)
    R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2013)
    R834799C001 (2014)
    R834799C001 (2015)
    R834799C001 (Final)
  • Abstract from PubMed
  • Full-text: Science Direct-Full Text HTML
    Exit
  • Abstract: Science Direct-Abstract
    Exit
  • Other: Science Direct-Full Text PDF
    Exit
  • Journal Article Verma V, Fang T, Guo H, King L, Bates JT, Peltier RE, Edgerton E, Russell AG, Weber RJ. Reactive oxygen species associated with water-soluble PM2.5 in the southeastern United States: spatiotemporal trends and source apportionment. Atmospheric Chemistry and Physics 2014;14(23):12915-12930. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Other: Harvard University-Abstract
    Exit
  • Journal Article Verma V, Fang T, Xu L, Peltier RE, Russell AG, Ng NL, Weber RJ. Organic aerosols associated with the generation of reactive oxygen species (ROS) by water-soluble PM2.5. Environmental Science & Technology 2015;49(7):4646-4656. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
  • Full-text from PubMed
  • Full-text: ES&T-Full Text HTML
    Exit
  • Abstract: ES&T-Abstract
    Exit
  • Other: ES&T-Full Text PDF
    Exit
  • Journal Article Verma V, Wang Y, El-Afifi R, Fang T, Rowland J, Russell AG, Weber RJ. Fractionating ambient humic-like substances (HULIS) for their reactive oxygen species activity—assessing the importance of quinones and atmospheric aging. Atmospheric Environment 2015;120:351-359. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (Final)
  • Full-text: ScienceDIrect-Full Text HTML
    Exit
  • Abstract: ScienceDIrect-Abstract
    Exit
  • Other: ScienceDIrect-Full Text PDF
    Exit
  • Journal Article Weber RJ, Guo H, Russell AG, Nenes A. High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years. Nature Geoscience 2016;9:282-285. R834799 (2016)
    R834799 (Final)
    R834799C001 (Final)
    R835410 (2013)
  • Full-text: Georgia Tech-Prepublication PDF
    Exit
  • Abstract: Nature-Abstract
    Exit
  • Journal Article Xu L, Guo H, Boyd CM, Klein M, Bougiatioti A, Cerully KM, Hite JR, Isaacman-VanWertz G, Kreisberg NM, Knote C, Olson K, Koss A, Goldstein AH, Hering SV, de Gouw JA, Baumann K, Lee S-H, Nenes A, Weber RJ, Ng NL. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States. Proceedings of the National Academy of Sciences of the United States of America 2015;112(1):37-42. R834799 (2015)
    R834799 (2016)
    R834799 (Final)
    R834799C001 (2015)
    R834799C001 (Final)
    R835403 (2014)
    R835403 (2015)
    R835403 (Final)
    R835410 (2013)
  • Full-text from PubMed
  • Abstract from PubMed
  • Associated PubMed link
  • Full-text: PNAS-Full-text PDF
    Exit
  • Abstract: PNAS-Abstract & Full-text HTML
    Exit
  • Supplemental Keywords:

    reactive oxygen species, ROS, oxidative stress, oxidative potential, Health, Scientific Discipline, Health Risk Assessment, Risk Assessments, Biochemistry, Environmental Monitoring, particulate matter, children's health, ambient air monitoring, climate change, air pollution, ambient particle health effects, airshed modeling, human health risk

    Relevant Websites:

    www.scape.gatech.edu Exit

    Progress and Final Reports:

    Original Abstract
  • 2011
  • 2012 Progress Report
  • 2013 Progress Report
  • 2014 Progress Report
  • 2015 Progress Report

  • Main Center Abstract and Reports:

    R834799    The Southeastern Center for Air Pollution and Epidemiology: Multiscale Measurements and Modeling of Mixtures

    Subprojects under this Center: (EPA does not fund or establish subprojects; EPA awards and manages the overall grant for this center).
    R834799C001 Development and Deployment of an Instrumentation Suite for Comprehensive Air Quality Characterization Including Aerosol ROS
    R834799C002 Examining In-Vehicle Pollution and Oxidative Stress in a Cohort of Daily Commuters
    R834799C003 Novel Estimates of Pollutant Mixtures and Pediatric Health in Two Birth Cohorts
    R834799C004 A Multi-City Time-Series Study of Pollutant Mixtures and Acute Morbidity