Source characterization and identification by real-time single particle mass spectrometry.

Abstract A Real-Time Single Particle Mass Spectrometer, RSMS-3, was deployed to Wilmington, Delaware to study regional and local contributions to fine and ultra-fine urban particulate matter (PM). Approximately two-thirds of PM1 consisted of internally mixed secondary aerosol. The remaining one-third was externally mixed including biomass burning (13%), fossil fuel combustion (7%) and various industrial sources (13%). In this last group, particle classes containing specific combinations of transition and/or heavy metals gave wind-rose plots consistent with specific point sources. For example, particles containing V and Ni were detected from different wind directions than those containing V and Fe. Samples from two industrial emission stacks, a steel manufacturing facility 10 km away and a coal-fired electrical power generation facility 5 km away, were analyzed and compared to the ambient data set. In each case, a direct correlation was found: a Pb–Zn–K–Na class for the steel manufacturing facility and an Fe–La/Ce class for the power generation facility. The ambient particle classes showed additional small signals from secondary components indicating atmospheric processing. Ambient particle classes containing only a subset of these elements, such as Zn only, Fe only and Pb–K only, were nonspecific, that is, the wind-rose plots were more diffuse and the particles could not be mapped to individual sources. The merits of stack sampling as an aid to interpreting single particle data sets are discussed.

[1]  A. Wexler,et al.  Field evaluation of the versatile aerosol concentration enrichment system (VACES) particle concentrator coupled to the rapid single-particle mass spectrometer (RSMS-3) , 2005 .

[2]  Tomas Baer,et al.  Aerosol mass spectrometry: An introductory review , 2006 .

[3]  D. Murphy,et al.  The design of single particle laser mass spectrometers. , 2007, Mass spectrometry reviews.

[4]  A. Wexler,et al.  The character of single particle sulfate in Baltimore , 2004 .

[5]  M. Johnston.  Sampling and analysis of individual particles by aerosol mass spectrometry. , 2000, Journal of mass spectrometry : JMS.

[6]  A. Wexler,et al.  Number concentrations of fine and ultrafine particles containing metals , 2004 .

[7]  C. Stanier,et al.  An Algorithm for Combining Electrical Mobility and Aerodynamic Size Distributions Data when Measuring Ambient Aerosol Special Issue of Aerosol Science and Technology on Findings from the Fine Particulate Matter Supersites Program , 2004 .

[8]  A. Wexler,et al.  Where do particulate toxins reside ? An improved paradigm for the structure and dynamics of the urban mid-Atlantic aerosol , 1998 .

[9]  Noble,et al.  Real-time single particle mass spectrometry: a historical review of a quarter century of the chemical analysis of aerosols , 2000, Mass spectrometry reviews.

[10]  A S Wexler,et al.  Application of the ART-2a algorithm to laser ablation aerosol mass spectrometry of particle standards. , 2001, Analytical chemistry.

[11]  K. Prather,et al.  Simultaneous measurement of the effective density and chemical composition of ambient aerosol particles. , 2007, Environmental science & technology.

[12]  G E Gordon,et al.  Rare Earths: Atmospheric Signatures for Oil-Fired Power Plants and Refineries , 1985, Science.

[13]  A. Wexler,et al.  Size-resolved ultrafine particle composition analysis, 1. Atlanta , 2003 .

[14]  C. Sioutas,et al.  A new compact aerosol concentrator for use in conjunction with low flow-rate continuous aerosol instrumentation , 2005 .

[15]  Shankararaman Chellam,et al.  Lanthanum and lanthanides in atmospheric fine particles and their apportionment to refinery and petrochemical operations in Houston, TX , 2006 .

[16]  Carlos Alberto Mendes Moraes,et al.  Chemical, physical, structural and morphological characterization of the electric arc furnace dust. , 2006, Journal of hazardous materials.

[17]  Rajan K. Chakrabarty,et al.  Emissions from the laboratory combustion of wildland fuels: Particle morphology and size , 2006 .

[18]  D. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 1: Theory , 2004 .

[19]  A. Wexler,et al.  Distribution of lead in single atmospheric particles , 2007 .

[20]  A. Wexler,et al.  Size‐resolved fine and ultrafine particle composition in Baltimore, Maryland , 2005 .

[21]  Z. Ning,et al.  Field Validation of the New Miniature Versatile Aerosol Concentration Enrichment System (mVACES) , 2006 .

[22]  Detection of negative ions from individual ultrafine particles. , 2002, Analytical chemistry.

[23]  Size‐resolved ultrafine particle composition analysis 2. Houston , 2003 .

[24]  Zoran Ristovski,et al.  Relation between particle mass and number for submicrometer airborne particles , 1999 .

[25]  Ulf Kirchner,et al.  Identification of diesel exhaust particles at an Autobahn, urban and rural location using single-particle mass spectrometry , 2003 .

[26]  A. Wexler,et al.  Identification of sources of atmospheric PM at the Pittsburgh Supersite—Part II: Quantitative comparisons of single particle, particle number, and particle mass measurements , 2006 .

[27]  A. Wexler,et al.  Mass spectrometry of individual particles between 50 and 750 nm in diameter at the Baltimore Supersite. , 2003, Environmental science & technology.

[28]  D. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 2: Application to Combustion-Generated Soot Aerosols as a Function of Fuel Equivalence Ratio , 2004 .

[29]  A. Wexler,et al.  Speciation of size-resolved individual ultrafine particles in Pittsburgh, Pennsylvania , 2005 .

[30]  A. Wexler,et al.  Ultrafine nitrate particle events in Baltimore observed by real-time single particle mass spectrometry , 2004 .

[31]  M. Johnston,et al.  Size and composition biases on the detection of individual ultrafine particles by aerosol mass spectrometry , 2000 .

[32]  J. Jimenez,et al.  In situ concentration of semi-volatile aerosol using water-condensation technology , 2005 .

[33]  P. Bhave,et al.  Comparison of two methods for obtaining quantitative mass concentrations from aerosol time-of-flight mass spectrometry measurements. , 2006, Analytical chemistry.

[34]  K. Prather,et al.  Determination of single particle mass spectral signatures from heavy-duty diesel vehicle emissions for PM2.5 source apportionment , 2007 .

[35]  A. Wexler,et al.  Characterization of Short-Term Particulate Matter Events by Real-Time Single Particle Mass Spectrometry , 2006 .

[36]  P. Hopke,et al.  Real-Time Characterization of the Composition of Individual Particles Emitted From Ultrafine Particle Concentrators , 2006 .

[37]  Performance of a Single Ultrafine Particle Mass Spectrometer , 2002 .

[38]  Kimberly A Prather,et al.  Recent advances in our understanding of atmospheric chemistry and climate made possible by on-line aerosol analysis instrumentation. , 2005, Analytical chemistry.