For decades, soot has been modeled as fractal-like aggregates of nearly equiaxed spherules. Cluster-cluster aggregation simulations, starting from a population of primary particles, give rise to structures that closely match real aerosols of solid particles produced in flames. In such simulations, primary particle size is uncorrelated with aggregate size, as all aggregates contain primary particles drawn from the same population. Aerosol measurements have been interpreted with this geometric model. Examination of transmission electron micrographs of soot samples from various sources shows that primary particle sizes are not well mixed within an aerosol population. Larger aggregates tend to contain larger primary particles and the variation in size is much larger between aggregates than within aggregates. The soot sources considered here are all substantially not well-mixed (aircraft jet engine, inverted diffusion flame, gasoline direct injection engine, heavy-duty compression ignition engine). The observed variations in primary particle size can be explained if soot aggregates are formed and grew by coagulation in small zones of the combustion chamber, prior to dilution and transport (with minimal coagulation) to the sampling system.
The total climate, air quality, and health impact of aircraft black carbon (BC) emissions depend on quantity (mass and number concentration) as well as morphology (fractal dimension and surface area) of emitted BC aggregates. This study examines multiple BC emission metrics from a gas turbine with a double annular combustor, CFM56-5B4-2P. As a part of the SAMPLE III.2 campaign, concurrent measurements of particle mobility, particle mass, particle number concentration, and mass concentration, as well as collection of transmission electron microscopy (TEM) samples, allowed for characterization of the BC emissions. Mass-and number-based emission indices were strongly influenced by thrust setting during pilot combustion and ranged from <1 to 208 mg/kg-fuel and 3 £ £ 10 12 to 3 £ £ 10 16 particles/kg-fuel, respectively. Mobility measurements indicated that mean diameters ranged from 7 to 44 nm with a strong dependence on thrust during pilot-only combustion. Using aggregation and sintering theory with empirical effective density relationships, a power-law relationship between primary particle diameter and mobility diameter is presented. Mean primary particle diameter ranged from 6 to 19 nm; however, laserinduced incandescence (LII) and mass-mobility-calculated primary particle diameters demonstrated opposite trends with thrust setting. Similarly, mass-mobility-calculated aggregate mass specific surface area and LII-measured surface area were not in agreement, indicating both methods need further development and validation before use as quantitative indicators of primary particle diameter and mass-specific surface area.
The restructuring of monodisperse soot aggregates due to coatings of secondary organic aerosol (SOA) was investigated in a series of photo-oxidation chamber experiments. Soot aggregates were generated by one of three sources (an ethylene premixed burner, a methane inverted diffusion burner, or a diesel generator), treated by denuding, size-selected by a differential mobility analyzer, and injected into a smog chamber, where they were exposed to the photo-oxidation products of p-xylene, which partitioned to form SOA coatings. The evolution of aggregates from their initial to final morphologies was investigated in situ by mobility and mass measurements and ex situ by transmission electron microscopy. At a given initial aggregate mobility diameter, diesel aggregates are less dense and composed of smaller primary particles than those generated by the two burners, and they restructure to a smaller final mobility diameter. Remarkably, the final degrees of restructuring of aggregates from all three sources exhibit the same linear dependence on the number of primary particles per aggregate. The observed linear relationship, valid for the atmospherically relevant SOA coating investigated here, could allow modelers to predict the evolution of aggregate morphology based on a single property of the aggregates.
A centrifugal particle mass analyzer and a modified differential mobility spectrometer were used to measure the mass and mobility of particulate matter emitted by CFM56-5B4/2P, CFM56-7B26/3, and PW4000-100 gas turbine engine sources. The mass-mobility exponent of the particulate matter from the CFM56-5B4/2P engine ranged from 2.68 to 2.82, whereas the effective particle densities varied from 600 to 1250 kg∕m 3 , depending on the static engine thrust and sampling methodology used. The effective particle densities from the CFM56-7B26/3 and PW4000-100 engines also fell within this range. The sample was conditioned with or without a catalytic stripper and with or without dilution, which caused the effective density to change, indicating the presence of condensed semivolatile material on the particles. Variability of the determined effective densities across different engine thrusts, based on the scattering about the line of best fit, was lowest for the diluted samples and highest for the undiluted sample without a catalytic stripper. This variability indicates that the relative amount of semivolatile material produced was engine thrust dependent. It was found that the nonvolatile particulate matter, effective particle density (in kilograms per cubic meter) of the CFM56-5B4/2P engine at relative thrusts below 30% could be approximated using the particle mobility diameter (d me in meters) with 11.92d 2.76−3 me . Nomenclature C = mass-mobility scaling component D m = mass-mobility exponent d me = particle mobility diameter k = mass-mobility prefactor M = suspended particle mass concentration m = particle mass n = particle number concentration
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