2015 Progress 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
Current 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
Project Period Covered by this Report: August 1, 2014 through July 31,2015
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 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.

Progress Summary:

During this reporting period, work has focused on data analyses, publishing papers, and two laboratory projects.

Laboratory work was undertaken in two areas: the development of an online ROS measurement system and analysis of the stability of ROS on archived filters.

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, a better assessment of variability in ROS and what drives it, and an assessment of possible artifacts associated with filter-based methods. In the past year, progress has been made on developing the method. First, an analysis was made to determine how to improve the sensitivity of the filter DTT-protocol for the much lower concentrations associated with an online particle collection system. Based on these results a method was developed involving a Particle Into Liquid Sample and flow injection system. The instrument was constructed and deployed for more than 2 months of ambient sampling. Filter samples were collected at the same time, extracted in water, and DTT measured. Overall, poor comparison was found between the online and filter results. Our hypothesis is that the online system is measuring closer to total DTT, whereas the filter system is measuring only the water-soluble fraction of DTT. To assess this, we plan to develop a method to measure total DTT of particles collected on filters and rerun the comparison (see future plans).

Stability of ROS on Filters: Linking ROS to health-endpoints through epidemiological analysis requires knowledge of ROS over an extended period of time. Because our approach is a retrospective analysis, ROS (DTT) data from the JST site was estimated based on a source apportionment analysis. 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 more than 2 years. We found that the DTT on archived filters was highly correlated to DTT measured immediately after filters were deployed, but lower by roughly 60%. Chemical speciation analysis suggests that this is due to loss of DTT activity of the organic fraction contributing to DTT (hydrophobic fraction), whereas the redox metals contributing to DTT activity were more stable (hydrophilic fraction). A manuscript on this work currently is being prepared.

Future Activities:

A goal for the next reporting period is to complete the following manuscripts:

  1. King, et al. Chemiluminescence measurements of NOx and NO versus cavity ring down NO2 at various sites in the southeastern United States.
  2. King, et al. On the spatial and seasonal distribution of a suite of air quality parameters based on paired measurements to investigate roadway emissions.
  3. Devlin, Verma, et al. PM generated ROS species associated with biological changes in humans exposed to fine concentrated air pollutants.
  4. Verma, et al. Overall summary of project finding on ROS measured by the DTT assay: sources, atmospheric processing, and health impacts.
  5. Fang, et al. Online measurements of ROS via the DTT assay.
  6. Gao, et al. Stability of ROS on archived filters.

Depending on availability of funds the following research areas will be explored:

  1. Online ROS system: We will continue to work on development of the online DTT instrument. In the next year, we plan to assess and verify the instrument performance by comparing with filter measurements of total DTT.
  2. To date, our work has focused on the water- and methanol-soluble components that contribute to fine particle ROS. Other studies have shown that solid particles, especially soot, also can be effective at generating ROS and are highly DTT active. The approach would be to modify the automated DTT/AA analysis system so that the redox chemistry can be done on an immersed filter, instead of in the filter extract. The system will be assessed by comparison to published diesel exhaust DTT intrinsic activities and contrasts between roadside to other sites (comparison between sites with high EC versus low EC concentrations). This area of research was proposed in last year’s report but was not pursued due to lack of funding. The plan is to revisit the problem in the next year.


Journal Articles on this Report : 11 Displayed | Download in RIS Format

Other subproject views: All 62 publications 17 publications in selected types All 17 journal articles
Other center views: All 334 publications 136 publications in selected types All 132 journal articles
Type Citation Sub Project Document Sources
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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • 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)
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  • Supplemental Keywords:

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

    Relevant Websites:

    Southeastern Center for Air Pollution & Epidemiology - Emory/Georgia Tech EPA Clean Air Research Center Exit

    Progress and Final Reports:

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