Zhang, Dan (2003-05). Laboratory investigation of chemical and physical properties of soot-containing aerosols. Doctoral Dissertation. Thesis uri icon

abstract

  • Soot particles released from fossil fuel combustion and biomass burning have a large impact on the regional/global climate by altering the atmospheric radiative properties and by serving as cloud condensation nuclei (CCN). However, the exact forcing is affected by the mixing of soot with other aerosol constituents, such as sulfuric acid. In this work, experimental studies have been carried out focusing on three integral parts: (1) heterogeneous uptake of sulfuric acid on soot; (2) hygroscopic growth of H2SO4-coated soot aerosols; (3) effect of H2SO4 coating on scattering and extinction properties of soot particles. A low-pressure laminar-flow reactor, coupled to ion driftchemical ionization mass spectrometry (ID-CIMS) detection, is used to study uptake coefficients of H2SO4 on combustion soot. The results suggest that uptake of H2SO4 takes place efficiently on soot particles, representing an important route to convert hydrophobic soot to hydrophilic aerosols. A tandem differential mobility analyzing (TDMA) system is employed to determine the hygroscopicity of freshly generated soot in the presence of H2SO4 coating. It is found that fresh soot particles are highly hydrophobic, while coating of H2SO4 significantly facilitates water uptake on soot even at sub-saturation relative humidities. The results indicate that aged soot particles in the atmosphere can potentially be an efficient source of CCN. Scattering and extinction coefficient measurements of the soot-H2SO4 mixed particles are conducted using a threewavelength Nephelometer and a multi-path extinction cell. Coating of H2SO4 is found to increase the single scattering albedo (SSA) of soot particles which has impact on the aerosol direct radiative effect. Other laboratory techniques such as transmission electron microscopy (TEM) and Fourier transform infrared spectrometry (FTIR) are utilized to examine the morphology and chemical composition of the soot-H2SO4 particles. This work provides critical information concerning the heterogeneous interaction of soot and sulfuric acid, and how their mixing affects the hygroscopic and optical properties of soot. The results will improve our ability to model and assess the soot direct and indirect forcing and hence enhance our understanding of the impact of anthropogenic activities on the climate.
  • Soot particles released from fossil fuel combustion and biomass burning have a
    large impact on the regional/global climate by altering the atmospheric radiative
    properties and by serving as cloud condensation nuclei (CCN). However, the exact
    forcing is affected by the mixing of soot with other aerosol constituents, such as sulfuric
    acid. In this work, experimental studies have been carried out focusing on three integral
    parts: (1) heterogeneous uptake of sulfuric acid on soot; (2) hygroscopic growth of
    H2SO4-coated soot aerosols; (3) effect of H2SO4 coating on scattering and extinction
    properties of soot particles. A low-pressure laminar-flow reactor, coupled to ion driftchemical
    ionization mass spectrometry (ID-CIMS) detection, is used to study uptake
    coefficients of H2SO4 on combustion soot. The results suggest that uptake of H2SO4
    takes place efficiently on soot particles, representing an important route to convert
    hydrophobic soot to hydrophilic aerosols. A tandem differential mobility analyzing
    (TDMA) system is employed to determine the hygroscopicity of freshly generated soot
    in the presence of H2SO4 coating. It is found that fresh soot particles are highly
    hydrophobic, while coating of H2SO4 significantly facilitates water uptake on soot even
    at sub-saturation relative humidities. The results indicate that aged soot particles in the atmosphere can potentially be an efficient source of CCN. Scattering and extinction
    coefficient measurements of the soot-H2SO4 mixed particles are conducted using a threewavelength
    Nephelometer and a multi-path extinction cell. Coating of H2SO4 is found to
    increase the single scattering albedo (SSA) of soot particles which has impact on the
    aerosol direct radiative effect. Other laboratory techniques such as transmission electron
    microscopy (TEM) and Fourier transform infrared spectrometry (FTIR) are utilized to
    examine the morphology and chemical composition of the soot-H2SO4 particles.
    This work provides critical information concerning the heterogeneous interaction
    of soot and sulfuric acid, and how their mixing affects the hygroscopic and optical
    properties of soot. The results will improve our ability to model and assess the soot
    direct and indirect forcing and hence enhance our understanding of the impact of
    anthropogenic activities on the climate.

ETD Chair

publication date

  • May 2003