2005 Progress Report: Aethalometric Liquid Chromatographic Mass Spectrometric Instrument

EPA Grant Number: R831074
Title: Aethalometric Liquid Chromatographic Mass Spectrometric Instrument
Investigators: Dasgupta, Purnendu K.
Institution: Towson University
Current Institution: The University of Texas at Arlington
EPA Project Officer: Chung, Serena
Project Period: September 1, 2003 through December 31, 2007 (Extended to December 31, 2008)
Project Period Covered by this Report: September 1, 2004 through December 31, 2005
Project Amount: $450,000
RFA: Measurement, Modeling, and Analysis Methods for Airborne Carbonaceous Fine Particulate Matter (PM2.5) (2003) RFA Text |  Recipients Lists
Research Category: Air , Air Quality and Air Toxics , Particulate Matter

Objective:

The objective of this research project is to fabricate, evaluate, and field test new instrumentation that can provide more information on the speciation of carbonaceous compounds in the atmosphere.

Progress Summary:

A membrane-based denuder coupled particle collector and ion analysis system was built and deployed in Bondville, Illinois. This instrument provides information on all major ionogenic gas composition and corresponding particle anionic compositions plus ammonium. Unlike previous instruments of this type, this instrument determines not only inorganic gases and particles, it also provides measures of acetic, formic, and oxalic acids and the corresponding particle phase organic acid anions, including methanesulfonate. This instrument provides 40 minute time resolution, performs gradient ion chromatography, has a small foot print, and uses a modest sampling rate of 1.5 liters per minute and still attains limits of detection in the low ng/m3 range. Dionex Corporation has licensed marketing rights of the membrane denuder used in this instrument from Texas Tech University (U.S. Patent 6,890,372).

A second copy of the above instrument was deployed in Beltsville, Maryland, for approximately 3 weeks and compared with two commercial monitoring instruments for aerosols and gases (MARGA instruments) being evaluated by the U.S. Environmental Protection Agency.

For a number of high-volume filter samples, the total carbon content was determined by elemental analysis techniques (combustion to CO2), and sequential solvent extraction liquid chromatography-mass spectrometry (LC-MS) was attempted to determine the percent of carbon that could be accounted for. In most cases, more than 50 percent of the carbon was unaccounted for suggesting this will not be a viable technique.

A membrane-based device was developed last year. This microvolume device removes CO2 near-quantitatively from an aqueous stream. This has been commercialized by Dionex Corporation and already has found considerable consumer acceptance.

A size selective multiple wavelength aethalometer has been developed. A 12 element LED-array ranging from 375-855 nm and a 512 element photodiode array are used. The geometry permits both spectral measurement of the particles and the size distribution measurement of the particles.

We have developed a means to classify water-soluble and insoluble carbon based on the ease with which it is oxidized to CO2 by liquid phase radical and photooxidation processes.

Future Activities:

We intend to carry out some work to complete the research on the ability of elemental versus organic carbon to convert NO2 into nitrous acid. The comparison with MARGA instruments will be written up. Efforts toward a movable, self-advancing tape-based size-discriminating multiwavelength aethalometer will continue. Mathematical deconvolution efforts to translate the raw data into particle size will be undertaken. Conversion of NO2 to nitrous acid by soot derived from meaningful participation in field experiments will be sought. Basic research into classifying carbon on solution phase oxidation will continue.


Journal Articles on this Report : 5 Displayed | Download in RIS Format

Other project views: All 46 publications 22 publications in selected types All 22 journal articles
Type Citation Project Document Sources
Journal Article Dasgupta PK, Li J, Zhang G, Luke WT, McClenny WA, Stutz J, Fried A. Summertime ambient formaldehyde in five U.S. metropolitan areas:Nashville, Atlanta, Houston, Philadelphia, and Tampa. Environmental Science & Technology 2005;39(13):4767-4783. R831074 (2005)
R831074 (Final)
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  • Journal Article Li J, Dasgupta PK, Luke W. Measurement of gaseous and aqueous trace formaldehyde:revisiting the pentanedione reaction and field applications. Analytica Chimica Acta 2005;531(1):51-68. R831074 (2005)
    R831074 (Final)
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  • Journal Article Ullah SMR, Williams A, Dasgupta PK. Automated low-pressure carbonate eluent ion chromatography system with postsuppressor carbon dioxide removal for the analysis of atmospheric gases and particles. Aerosol Science and Technology 2005;39(11):1072-1084. R831074 (2005)
    R831074 (2006)
    R831074 (2007)
    R831074 (Final)
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  • Journal Article Takeuchi M, Rahmat Ullah SM, Dasgupta PK, Collins DR, Williams A. Continuous collection of soluble atmospheric particles with a wetted hydrophilic filter. Analytical Chemistry 2005;77(24):8031-8040. R831074 (2005)
    R831074 (2006)
    R831074 (Final)
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  • Journal Article Ullah SMR, Adams RL, Srinivasan K, Dasgupta PK. Asymmetric membrane-fiber based carbon dioxide removal devices for ion chromatography. Analytical Chemistry 2004;76(23):7084-7093. R831074 (2005)
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  • Supplemental Keywords:

    aethalometry, ion chromatography, liquid chromatography, carbonaceous particles, atmospheric aerosols, oxidation to CO2, membrane transfer, conductometry,, RFA, Health, Scientific Discipline, PHYSICAL ASPECTS, Air, Ecosystem Protection/Environmental Exposure & Risk, particulate matter, Air Quality, air toxics, Environmental Chemistry, Air Pollution Effects, Risk Assessments, Monitoring/Modeling, Analytical Chemistry, Environmental Monitoring, Physical Processes, Engineering, Chemistry, & Physics, Environmental Engineering, air quality modeling, health effects, particle size, carbon aerosols, atmospheric particulate matter, human health effects, PM 2.5, atmospheric particles, aerosol particles, mass spectrometry, ambient air monitoring, air quality models, exposure, air modeling, emissions, thermal desorption, molecular markers, gas chromatography, air sampling, carbon particles, air quality model, human exposure, ambient particle health effects, particulate matter mass, aethalometric liquid chromatographic mass spectrometry, aersol particles, monitoring of organic particulate matter, aerosol analyzers, human health risk, measurement methods

    Relevant Websites:

    http://www.depts.ttu.edu/chemistry/faculty/dasgupta/dasgupta.html Exit

    Progress and Final Reports:

    Original Abstract
  • 2004 Progress Report
  • 2006 Progress Report
  • 2007 Progress Report
  • 2008 Progress Report
  • Final Report