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

Composition, shape factor, size, and fractal dimension of soot aerosol particles generated in a propane/O2, flame were determined as a function of the fuel equivalence ratio (φ). Soot particles were first size-selected by a differential mobility analyzer (DMA) and then analyzed by an Aerodyne aerosol mass spectrometer (AMS). The DMA provides particles of known mobility diameter (dm ). The AMS quantitatively measures the mass spectrum of the nonrefractory components of the particles and also provides the vacuum aerodynamic diam eter (dva ) corresponding to the particles of known mobility diameter. The measured dm, dva , and nonrefractory composition are used in a system of equations based on the formulation presented in the companion article to estimate the particle dynamic shape factor, total mass, and black carbon (BC) content. Fractal dimension was estimated based on the mass-mobility relationship. Two types of soot particles were observed depending on the fuel equivalence ratio. Type 1: for φ < 4 (lower propane/O2), dva ; was nearly constant and independent of dm . The value of dva increased with increasing φ. Analysis of the governing equations showed that these particles were highly irregular (likely fractal aggregates), with a dynamic shape factor that increased with dm and φ. The fractal dimension of these particles was approximately 1.7. These particles were composed mostly of BC, with the organic carbon content increasing as φ increased. At φ = 1.85, the particles were about 90% BC, 5% PAH, and 5% aliphatic hydrocarbon (particle density = 1.80 g/cm3). Type 2: for φ > 4 (high propane/O2), dva was linearly proportional to dm . Analysis of the governing equations showed that these particles were nearly spherical (likely compact aggregates), with a dynamic shape factor of 1.1 (versus 1 for a sphere) and a fr actal dimension of 2.95 (3 for a sphere). These particles were composed of about 50% PAH, 45% BC, and 5% aliphatic hydrocarbons (particle density = 1.50 g/cm3). These results help interpret some measurement s obtained in recent field studies.

[1]  Qi Zhang,et al.  Time- and size-resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes , 2005 .

[2]  P. Mcmurry,et al.  Structural Properties of Diesel Exhaust Particles Measured by Transmission Electron Microscopy (TEM): Relationships to Particle Mass and Mobility , 2004 .

[3]  P. Mcmurry,et al.  Measurement of Inherent Material Density of Nanoparticle Agglomerates , 2004 .

[4]  Kenneth A. Smith,et al.  Numerical Characterization of Particle Beam Collimation: Part II Integrated Aerodynamic-Lens–Nozzle System , 2004 .

[5]  Charles E. Kolb,et al.  Chase Studies of Particulate Emissions from in-use New York City Vehicles , 2004 .

[6]  Jacob A. Moulijn,et al.  Measuring diesel soot with a scanning mobility particle sizer and an electrical low-pressure impactor: Performance assessment with a model for fractal-like agglomerates , 2004 .

[7]  Ilan Koren,et al.  Measurement of the Effect of Amazon Smoke on Inhibition of Cloud Formation , 2004, Science.

[8]  J. Hansen,et al.  Soot climate forcing via snow and ice albedos. , 2004, Proceedings of the National Academy of Sciences of the United States of America.

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

[10]  J. Seinfeld,et al.  Correction to “New particle formation from photooxidation of diiodomethane (CH2I2)” , 2003 .

[11]  J. Seinfeld,et al.  Aircraft‐based aerosol size and composition measurements during ACE‐Asia using an Aerodyne aerosol mass spectrometer , 2003 .

[12]  J. Seinfeld,et al.  New particle formation from photooxidation of diiodomethane (CH2I2) , 2003 .

[13]  Makiko Sato,et al.  Global atmospheric black carbon inferred from AERONET , 2003, Proceedings of the National Academy of Sciences of the United States of America.

[14]  Charles E. Kolb,et al.  Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer , 2003 .

[15]  Martin Gallagher,et al.  2. Measurements of fine particulate chemical composition in two U.K. cities , 2003 .

[16]  Hugh Coe,et al.  Quantitative sampling using an Aerodyne aerosol mass spectrometer 1. Techniques of data interpretation and error analysis , 2003 .

[17]  P. Mcmurry,et al.  Relationship between particle mass and mobility for diesel exhaust particles. , 2003, Environmental science & technology.

[18]  J. Seinfeld,et al.  New particle formation from photooxidation of diiodomethane ( CH 2 I 2 ) , 2003 .

[19]  J. Hansen,et al.  Climate Effects of Black Carbon Aerosols in China and India , 2002, Science.

[20]  Charles E. Kolb,et al.  A Numerical Characterization of Particle Beam Collimation by an Aerodynamic Lens-Nozzle System: Part I. An Individual Lens or Nozzle , 2002 .

[21]  Xin Wang,et al.  The Relationship between Mass and Mobility for Atmospheric Particles: A New Technique for Measuring Particle Density , 2002 .

[22]  E. Feil,et al.  Climate Effects of Black Carbon Aerosols in China and India , 2002 .

[23]  V. Ramanathan,et al.  Aerosols, Climate, and the Hydrological Cycle , 2001, Science.

[24]  Joachim V. R. Heberlein,et al.  Thermal plasma deposition of nanophase hard coatings , 2001 .

[25]  J. Lelieveld,et al.  The Indian Ocean Experiment: Widespread Air Pollution from South and Southeast Asia , 2001, Science.

[26]  M. Jacobson,et al.  Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols , 2022 .

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

[28]  P. Ziemann,et al.  Real-Time Chemical Analysis of Organic Aerosols Using a Thermal Desorption Particle Beam Mass Spectrometer , 2000 .

[29]  Kenneth A. Smith,et al.  Development of an Aerosol Mass Spectrometer for Size and Composition Analysis of Submicron Particles , 2000 .

[30]  P. Buseck,et al.  Soot and sulfate aerosol particles in the remote marine troposphere , 1999 .

[31]  R. Flagan On Differential Mobility Analyzer Resolution , 1999 .

[32]  Robert A. Fletcher,et al.  The evolution of soot precursor particles in a diffusion flame , 1998 .

[33]  Kenneth A. Smith,et al.  Aerosol mass spectrometer for size and composition analysis of submicron particles , 1998 .

[34]  S. Pandis,et al.  A study of the ability of pure secondary organic aerosol to act as cloud condensation nuclei , 1997 .

[35]  Christopher M. Sorensen,et al.  The Morphology of Macroscopic Soot , 1996 .

[36]  J. Seinfeld,et al.  Dynamics of Tropospheric Aerosols , 1995 .

[37]  David B. Kittelson,et al.  Generating Particle Beams of Controlled Dimensions and Divergence: I. Theory of Particle Motion in Aerodynamic Lenses and Nozzle Expansions , 1995 .

[38]  Peng Liu,et al.  Generating Particle Beams of Controlled Dimensions and Divergence: II. Experimental Evaluation of Particle Motion in Aerodynamic Lenses and Nozzle Expansions , 1995 .

[39]  Henning Bockhorn,et al.  Soot Formation in Combustion: Mechanisms and Models , 1994 .

[40]  Henning Bockhorn,et al.  Soot Formation in Combustion , 1994 .

[41]  T. Kashiwagi,et al.  Comparisons of Soot Volume Fraction Measurements Using Optical and Isokinetic Sampling Techniques | NIST , 1993 .

[42]  J. Penner,et al.  Large contribution of organic aerosols to cloud-condensation-nuclei concentrations , 1993, Nature.

[43]  W. M. Haynes CRC Handbook of Chemistry and Physics , 1990 .

[44]  U. Baltensperger,et al.  Scaling behaviour of physical parameters describing agglomerates , 1990 .

[45]  B. Albrecht Aerosols, Cloud Microphysics, and Fractional Cloudiness , 1989, Science.

[46]  G. Cass,et al.  Characteristics of summer midday low-visibility events in the Los Angeles area , 1989 .

[47]  F. Rodríguez-Reinoso,et al.  Chemistry and Physics of Carbon , 2022 .

[48]  G. Cass,et al.  Characteristics of atmospheric organic and elemental carbon particle concentrations in Los Angeles. , 1986, Environmental science & technology.

[49]  Otto G. Raabe,et al.  Slip correction measurements of spherical solid aerosol particles in an improved Millikan apparatus , 1985 .

[50]  Stephen E. Stein,et al.  Detailed kinetic modeling of soot formation in shock-tube pyrolysis of acetylene , 1985 .

[51]  T. L. Wolfe,et al.  An assessment of the impact of pollution on global cloud albedo , 1984 .

[52]  O. Raabe,et al.  Re-evaluation of millikan's oil drop data for the motion of small particles in air , 1982 .

[53]  Owen I. Smith,et al.  Fundamentals of soot formation in flames with application to diesel engine particulate emissions , 1981 .

[54]  Y. Manheimer-Timnat,et al.  Sooting Behavior of Gaseous Hydrocarbon Diffusion Flames and the Influence of Additives , 1980 .

[55]  R. C. Weast CRC Handbook of Chemistry and Physics , 1973 .

[56]  E. M. Bulewicz Combustion , 1964, Nature.

[57]  R. Millikan NON-EQUILIBRIUM SOOT FORMATION IN PREMIXED FLAMES , 1962 .

[58]  D'arcy W. Thompson On Growth and Form , 1917, Nature.

[59]  D'arcy W. Thompson,et al.  On Growth and Form , 1917, Nature.