“…14,[181][182][183][184] The ratio of carbon sp 2 -to-sp 3 bond hybridization increases with the size of the crystallite-layer planes, while the interlayer spacing decreases to approach that of graphite. 113,141,[183][184][185][186][187] Graphitization involves the scavenging of interstitial carbon atoms from between layer planes, lateral crystallite growth, and bond rearrangement. 183,188 Some carbonaceous materials, including some forms of turbostratic graphite, are non-graphitizing, i.e.…”
Section: Chemical Evolutionmentioning
confidence: 99%
“…they cannot undergo full graphitization to the most ordered form of graphite. [181][182][183][184]186,187,189,190 Carbonization: Carbonization is the pyrolytic conversion of hydrocarbon species and substituted hydrocarbons towards elemental carbon (i.e., pure carbon). It is marked by an increase in the carbon-to-hydrogen (C/H) ratio.…”
This paper presents a glossary and review of terminology used to describe the chemical and physical processes involved in soot formation and evolution. This review is intended to aid in communication within the field and across disciplines. There are large gaps in our understanding of soot formation and evolution and inconsistencies in the language used to describe the associated mechanisms. These inconsistencies lead to confusion within the field and hinder progress in addressing the gaps in our understanding. This review provides a list of definitions of terms and presents a description of their historical usage. It also addresses the inconsistencies in the use of terminology in order to dispel confusion and facilitate the advancement of our understanding of soot chemistry and particle characteristics. The intended audience includes senior and junior members of the soot, black-carbon, brown-carbon, and carbon-black scientific communities, researchers new to the field, and scientists and engineers in associated fields with an interest in carbonaceous-material production via high-temperature hydrocarbon chemistry.
“…14,[181][182][183][184] The ratio of carbon sp 2 -to-sp 3 bond hybridization increases with the size of the crystallite-layer planes, while the interlayer spacing decreases to approach that of graphite. 113,141,[183][184][185][186][187] Graphitization involves the scavenging of interstitial carbon atoms from between layer planes, lateral crystallite growth, and bond rearrangement. 183,188 Some carbonaceous materials, including some forms of turbostratic graphite, are non-graphitizing, i.e.…”
Section: Chemical Evolutionmentioning
confidence: 99%
“…they cannot undergo full graphitization to the most ordered form of graphite. [181][182][183][184]186,187,189,190 Carbonization: Carbonization is the pyrolytic conversion of hydrocarbon species and substituted hydrocarbons towards elemental carbon (i.e., pure carbon). It is marked by an increase in the carbon-to-hydrogen (C/H) ratio.…”
This paper presents a glossary and review of terminology used to describe the chemical and physical processes involved in soot formation and evolution. This review is intended to aid in communication within the field and across disciplines. There are large gaps in our understanding of soot formation and evolution and inconsistencies in the language used to describe the associated mechanisms. These inconsistencies lead to confusion within the field and hinder progress in addressing the gaps in our understanding. This review provides a list of definitions of terms and presents a description of their historical usage. It also addresses the inconsistencies in the use of terminology in order to dispel confusion and facilitate the advancement of our understanding of soot chemistry and particle characteristics. The intended audience includes senior and junior members of the soot, black-carbon, brown-carbon, and carbon-black scientific communities, researchers new to the field, and scientists and engineers in associated fields with an interest in carbonaceous-material production via high-temperature hydrocarbon chemistry.
“…Soot sampled from 5 mm is rather nascent soot (Apicella et al, 2018) and an appropriate value for nascent soot is 1.5 g/cm 3 (Abid et al, 2008). Other effects which may influence the soot oxidation in our experiments, e.g., oxidation by other oxidants formed during the oxidation of sampled flame species like the OH radical or competitive particle growth, are not considered herein.…”
Section: Particle Size Distributions During the Oxidation Process Andmentioning
confidence: 99%
“…Even the aging of soot has an influence on its nanostructure, e.g., differences in surface microstructure of nascent soot and mature soot are known (Camacho et al, 2015), and can explain different reactivity for different types of soot. Apicella et al (2018) have shown by high resolution transmission electron microscopy (HRTEM) and energy loss spectroscopy (EELS) that nascent soot has a quite disordered and heterogeneous structure and relatively low concentrations of sp 2 hybridized carbon in comparison to young, intermediate, and mature soot presenting spherule aggregates.…”
Oxidation by molecular oxygen of freshly-produced soot from a flat ethylene-air-flame is investigated under well-controlled conditions in a flow reactor at 773-1273 K and atmospheric pressure. Soot particles are characterized before and after oxidation by electrical mobility technique. In addition to the size-classified soot number density, the molecular gasphase species are obtained simultaneously by molecular-beam mass spectrometry. Oxidation behavior of soot particles as well as some hydrocarbon species sampled from the soot source was determined quantitatively. Oxygenated species are formed as molecular intermediates during the oxidation process inside the reactor. Different particle size distributions have been investigated by varying the sampling position and equivalence ratio of the flame. Oxidation of soot starts at different temperatures, but is clearly separated from oxidation of flame species starting earlier at lower temperatures. Soot oxidation rates were calculated and comparison with the Nagle-Strickland-Constable model indicates that the investigated flamesampled soot is more reactive than graphite under the investigated conditions. The presented dataset may help to validate existing soot models.
“…Key to the development of strategies for the reduction of soot emissions, or for its capture/storage/removal is understanding the processes governing soot formation and oxidation. Research in this area includes characterization of fundamental chemical and physical properties of soot such as elemental composition [10], degree of graphitization [11], surface functional group chemistry [12], oxidative reactivity [13,14], carbon nanostructure [15,16], surface area [10,17], fractal geometry [18], and size [19].…”
Morphology plays an important role in determining behaviour and impact of soot nanoparticles, including effect on human health, atmospheric optical properties, contribution to engine wear, and role in marine ecology. However, its nanoscopic size has limited the ability to directly measure useful morphological parameters such as surface area and effective volume. Recently, 3D morphology characterization of soot nanoparticles via electron tomography has been the subject of several introductory studies. So-called '3D-TEM' has been posited as an improvement over traditional 2D-TEM characterization due to the elimination of the error-inducing information gap that exists between 3-dimensional soot structures and 2-dimensional TEM projections. Little follow-up work has been performed due to difficulties with developing methodologies into robust high-throughput techniques. Recent work by the authors has exhibited significant improvements in efficiency, though as yet due consideration has not been given to assessing fidelity of the technique. This is vital to confirm significant and tangible improvements in soot-characterization accuracy that will establish 3D-TEM as a legitimate tool. Synthetic ground-truth data was developed to closely mimic real soot structures and the 3D-TEM volume-reconstruction process. A variety of procedures were tested to assess the magnitude and nuances of deviations from ground-truth values. Results showed average Z-elongation due to the 'missing-wedge' at 3.5% for the previously developed optimized procedure. Mean deviations from ground-truth in volume and surface area were 2.0% and -0.1% respectively. Results indicate highly accurate 3D-reconstruction can be achieved with an optimized procedure that can bridge the gap to permit highthroughput 3D morphology characterization of soot.
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