Browsing by Subject "soot"
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Item Heterogeneous organic acid uptake on soot surfaces(2009-05-15) Levitt, Nicholas PaulAtmospheric particulates have been known to act as cloud condensation nuclei (CCN) and therefore their presence can indirectly affect important processes such as global radiation balance through cloud formation. Soot particles are well known to be atmospheric constituents, but the hydrophobic nature of fresh soot likely prohibits them from encouraging cloud development. Soot aged through contact with oxygenated organic compounds may become hydrophilic enough to promote water uptake. In this study I have observed the interaction between a number of carboxylic acids and soot from different fuel sources and formation mechanisms. A low pressure fast flow reactor was used to control the contact between the solid phase soot and gas phase organics, while chemical ionization-mass spectrometry was utilized to monitor concentrations of gas phase organics. Most acids irreversibly deposited on the soot surfaces, and the uptake coefficient was measured in the wide range of 9.0 x 10-4 to 1.0 x 10-1. The Brunauer, Emmett, and Teller (BET) surface areas of the soots were measured and the soot bulk and surface chemical compositions were investigated with Fourier transform infrared (FTIR) spectroscopy and attenuated total reflection (ATR) spectroscopy to help explain differences in uptake. By comparing the mono and dicarboxylic acids and the information gathered from soot physiochemical properties I have discussed possible uptake mechanisms.Item How Physical and Chemical Properties Change Ice Nucleation Efficiency of Soot and Polyaromatic Hydrocarbon Particles(2012-10-19) Suter, Katie AnnHeterogeneous freezing processes in which atmospheric aerosols act as ice nuclei (IN) cause nucleation of ice crystals in the atmosphere. Heterogeneous nucleation can occur through several freezing mechanisms, including contact and immersion freezing. The mechanism by which this freezing occurs depends on the ambient conditions and composition of the IN. Aerosol properties change through chemical aging and reactions with atmospheric oxidants such as ozone. We have conducted a series of laboratory experiments using an optical microscope apparatus equipped with a cooling stage to determine how chemical oxidation changes the ability of atmospheric aerosols to act as IN. Freezing temperatures are reported for aerosols composed of fresh and oxidized soot and polyaromatic hydrocarbons (PAHs) including anthracene, phenanthrene, and pyrene. Our results show that oxidized soot particles initiate ice freezing events at significantly warmer temperatures than fresh soot, 3 ?C on average. All oxidized PAHs studied had significantly warmer freezing temperatures than fresh samples. The chemical changes presumably causing the improved ice nucleation efficiency were observed using Fourier Transform Infrared Spectroscopy with Horizontal Attenuated Total Reflectance (FTIR-HATR). The addition of C=O bonds at the surface of the soot and PAHs led to changes in freezing temperatures. Finally, we have used classical nucleation theory to derive heterogeneous nucleation rates for the IN compositions in this research. The overall efficiency of the IN can be compared in order of least efficient to most efficient: fresh phenanthrene, fresh anthracene, fresh soot, oxidized phenanthrene, fresh pyrene, oxidized anthracene, oxidized soot, and oxidized pyrene. Overall oxidation of aerosols increases their ability to act as IN. Our results suggest that oxidation processes facilitate freezing at warmer temperatures at a broader range of conditions on the atmosphere.Item Investigation on Nitric Oxide and Soot of Biodiesel and Conventional Diesel using a Medium Duty Diesel Engine(2012-07-16) Song, HoseokBiodiesel has been suggested as an alternative fuel to the petroleum diesel fuel. It beneficially reduces regulated emission gases, but increases NOx (nitric oxide and nitrogen dioxide) Thus, the increase in NOx is the barrier for potential growth of the biodiesel fuel. In general, NOx formation is dominated by flame temperature. Interestingly, soot can play a role as a heat sink as well as a heat transfer media to high temperature gases. Thus, the cooling effect of soot may change the flame temperature and therefore, NOx emissions. In this study, emphasis is placed on the relationship between soot and NO (Nitric oxide) formation. For the experimental study, a metallic fuel additive is used since barium is known to be effective to suppress soot formation during combustion. The barium additive is applied to #2D (Number 2 diesel fuel) by volume basis: 0.1, 0.25 and 0.5 %-v, and to the palm olein oil by 0.25 %-v. All the tests are carried out in a four-cylinder medium duty diesel engine, 4045 DI diesel engine, manufactured by John Deere. For the analysis, an analytical model is used to estimate combustion temperature, NO concentration and soot emissivity. The results show that NO concentration does not have the expected trade-off relation with soot. Rather, NO concentration is found to be more strongly affected by ambient temperature and combustion characteristics than by soot. The results of the analytical model show the reasonable NO estimation and the improvement on temperature calculation. However, the model is not able to explain the detailed changes of soot emissivity by the different fuels since the emissivity correlation is developed empirically for diesel fuel.Item Laboratory investigation of chemical and physical properties of soot-containing aerosols(Texas A&M University, 2006-08-16) Zhang, DanSoot 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.Item Linking Chemical Changes in Soot and Polyaromatics to Cloud Droplet Formation(2010-01-14) Mason, Laura E.Soot and other products of incomplete combustion play an important role in the chemistry of the atmosphere. As particles are exposed to trace gases, such as ozone, their chemistry and physical properties can be altered leading to changes in their optical properties, as well as their cloud condensation nuclei and ice nucleation abilities. These alterations can lead to changes in the global radiative budget and cloud microphysical processes, which in turn affect the climate. In this study, the chemical and physical changes associated with the oxidation of pyrene, anthracene, and carbon (lampblack) by ozone were investigated. Fourier Transform Infrared Spectroscopy was used to identify oxidation products and track reaction progress for these representative aerosols. A C=O band attributed to a carboxylic acid formation was observed for all three substances, at each level of exposure to ozone - 20 ppm, 40 ppm, and 80 ppm. Second order reaction rate constants ranged from 9.58 x 10-16 cm2 molecules-1 s-1 to 7.71 x 10-13 cm2 molecules-1 s-1. Measurements of water uptake, ice nucleation efficiency, and optical properties were obtained to determine whether any physical changes associated with the oxidation process occurred. Optical measurements show an increase in the ultra-violet absorption of anthracene, but not for pyrene, while an increase in the visible absorption for pyrene was observed, but not for anthracene. Oxidized soot froze at a warmer temperature (-22.8 degrees C) then fresh soot (-25.6 degrees C), showing an increase in ice nucleation efficiency. Our data indicates that oxidation by ozone does alter the chemistry and physical properties of the substances study, leading to possible changes in how they interact with atmospheric processes.