Soot Nanostructure Research Articles

Plasma treatment on flame soot: view from nanostructure and reactivity of soot

In recent years, the use of plasma for pollutant emission control has an expected potential. In this study, soot particles from flames were sampled from an ethylene inverse diffusion flame, which were placed in a self-designed dielectric barrier discharge plasma device for reaction treatment. The nanostructure and oxidation reactivity of soot particles after plasma treatment were evaluated by transmission electron microscopy, Raman spectroscopy, X-ray diffraction analysis and X-ray photoelectron spectroscopy. With 16 kV, 2.5 kHz as an example, with the treatment of plasma, the fringe length decreases (1.3% and 9.6%), and the fringe tortuosity increases (1.1% and 8.7%) in both high-maturity and low-maturity soot particles, which means that the oxidation activity of soot is enhanced after plasma discharge. Raman spectra, X-ray diffraction analysis spectra and X-ray photoelectron spectroscopy spectra have confirmed this phenomenon, especially the oxidation activity of soot particles under the action of plasma at high maturity is more obvious. It is worth noting that the enhancement of soot oxidation activity after plasma discharge has certain limitations, that is, the oxidation activity will not continue to increase after it is enhanced to a certain intensity, which may be related to the selection of Ar as the atmosphere gas.

Oxidation-induced variations in the physical and fragmentation characteristics of exhaust soot from DMC-diesel blend: Effect of NO presence in the air atmosphere

This study investigated the changes in physical properties (including morphology, primary particle diameter, fractal dimension, and nanostructure) and fragmentation characteristics of exhaust soot from a modern direct injection diesel engine fueled with diesel (D100) and its blend with 7 vol% of dimethyl carbonate (DMC7) during oxidation processes in air and air-NO atmospheres. Soot particles (D100 soot and DMC7 soot) with specific oxidation degrees (0%, 20%, 50%, and 80%) were produced using a thermogravimetric analyzer, then applied to a high-resolution transmission electron microscopy to generate images. The results exhibited that the morphology for D100 soot and DMC7 soot transformed similarly through oxidation, experiencing an increase in fractal dimension, and a decrease in primary particle diameter, while the introduction of NO to the air accelerated these transformations. Additionally, the nanostructure of both soot particles was gradually ordered through oxidation, as evidenced by longer fringe length, narrower separation distance, and lower tortuosity, while DMC7 soot showed lower order degree compared to D100 soot. Interestingly, the ordering processes of soot nanostructure were decelerated as NO was involved in the oxidation process. Furthermore, the aggregate fragmentation rate for both soot particles declined over the oxidation process, while the possibility for primary particle fragmentation increased overall. Moreover, DMC7 soot exhibited significantly lower aggregate fragmentation rate and higher possibility for primary particle fragmentation than D100 soot at the same oxidation stage. This suggests that DMC7 soot is more susceptible to internal oxidation compared to D100 soot. Furthermore, the presence of NO in the air promoted aggregate fragmentation, while reducing the possibility of primary particle fragmentation.

Effects of ammonia addition on the soot nanostructure and oxidation reactivity in n-heptane/toluene diffusion flames

Co-firing NH3 with conventional hydrocarbon fuels is an important approach for reducing CO2 emissions in existing combustion systems. Besides CO2, the blending of NH3 would also notably affect soot formation and its oxidation behaviors. In the present study, we focus on the effects of NH3 on the nanostructure and oxidation characteristics of soot produced in diffusion flames of n-heptane/toluene mixtures. Two configurations of laminar co-flow diffusion flame, including both normal and inverse diffusion flames (NDF and IDFs), were used for investigation. High-resolution transmission electron microscopy (HRTEM), Raman spectroscopy (Raman), and Thermogravimetric analysis (TGA) were employed for soot characterization. The HRTEM and Raman spectra showed that with the increase of NH3 blending ratio, the fringe length (La) and the degree of graphitization decreased while the microcrystal tortuosity (Tf) increased. The results are in consistent with TGA analysis which suggests the promoting effects of NH3 on the soot oxidation reactivity. Difference between NDF and IDF with respect to the soot nanostructure and oxidation activity were discussed. It is our hope that the present results could deepen our understanding on the effects of NH3 on soot nanostructure and oxidation behavior and benefit the design of particulate filters for combustion devices fueled with hydrocarbon/NH3 mixtures.

Effect of co-combustion of coal with biomass on the morphology of soot

This study performed an experimental investigation to explore the effect of co-combustion of coal with biomass on the morphological parameters and nanostructure of soot. Three types of soot, namely Shenghua coal (SH) soot, Pinewood biomass (PW) soot, and Co-combustion of SH and PW (CC) soot, were collected from the combustion flames of Shenhua coal, Pinewood biomass, and a mixture of coal and biomass. Thereafter, the soot samples were observed and analyzed by means of transmission electron microscope (TEM) and scanning electron microscope (SEM) to obtain their morphological parameters and nanostructure characteristics. The TEM results showed that the size of nascent soot particles generated in co-combustion flame is the largest, rather than between the sizes of PW and SH soot. The nanostructure of the three types of soot primary particles is mainly composed of straight parallel crystal stripes. The separation distance of crystal stripes in SH soot was measured to be larger than that in PW soot, indicating that the crystal structure of soot generated in Pine biomass combustion flame is more compact. It was also observed that both coal-derived primary soot particles and biomass-derived primary soot particles were formed in the co-combustion flame. SEM results indicated that PW soot agglomerates have stronger aggregation performance and more compact structure then SH soot and CC soot. The primary particle size of SH and CC soot agglomerates was mainly concentrated between 50 and 70 nm, while that of PW soot agglomerates was relatively uniform. Furthermore, the number of primary particles in SH soot and CC soot was distributed over a wide range compared to PW soot.

Effects of polyoxymethylene dimethyl ethers (PODEn) on soot characteristics in isooctane inverse diffusion flames

Polyoxymethylene dimethyl ethers (PODEn, n = 1–3) such as dimethoxymethane (DMM) and PODE3 are considered highly promising alternative fuels due to their lack of C–C bonds and significant oxygen contents. Particularly, PODE3-blends with diesel have been proven to substantially reduce soot emissions and fuel consumption rates under optimized engine conditions, although the impact on soot nanostructure properties remains unclear. This study explored the effects of DMM and PODE3 on soot characteristics in isooctane (i-octane) inverse diffusion flames, focusing on soot morphology, soot nanostructure, soot nanocrystallite, and soot spectral features. To compare soot particles behavior, DMM and PODE3 blended as the isooctane substitute (by 20% and 40% volumetric fractions) were examined with various diagnostic techniques, including high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS).The results showed that DMM and PODE3 contributed to a reduction in sooting tendency from i-octane flames, whereas the average soot mass decreased significantly as the PODE3 ratio increased, consistent with a higher oxygen concentration. Therefore, 20% PODE3/i-octane exhibited growing disorganized arrangements of soot particles with shorter fringes, smaller crystallite sizes, and a relatively lower degree of graphitization than 20% and 40% DMM additions. However, XPS analysis indicated that soot produced from PODE3/i-octane mixtures had less oxygen atoms because PODE3 has multiple –CH2O- chain groups that can convert oxygen into carbon monoxide with little soot production. Moreover, HRTEM, XRD, and Raman spectra analyses of 40% PODE3-doped flames confirmed an exceptional correlation with turbostratic soot structure, as manifested by the shortest fringe length, longest fringe tortuosity, more amorphous soot with the smallest crystallite dimensions, and least degree of graphitization.

Effect of ammonia addition on nanostructure of soot in laminar coflow diffusion flames of ethylene diluted with nitrogen

The effect of ammonia addition on the nanostructure of soot particles was studied experimentally for ethylene diffusion flames. To compensate the thermal effect and nitrogen-containing species production when ammonia was added, the total mole fraction of ammonia and nitrogen was fixed in the fuel stream. Soot particle size, fringe length, and fringe tortuosity were measured through transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM). A complementary X-ray photoelectron spectroscopy (XPS) analysis provided information about the chemical bonding of soot. A significant delay in soot growth was observed and the particle size increased with the addition of ammonia. While there was no obvious correlation between the fractal dimension of soot and ammonia mole fraction (XNH3) or sampling location. With the addition of ammonia, the mean fringe length increased reasonably linearly with XNH3 and the fringe tortuosity increased up to XNH3 ≈ 0.17 and then decreased with XNH3, which suggested that ammonia addition led to higher graphitization and lower oxidative activity. The soot from ammonia diluted flame exhibited lower reactivity, implying the delay of soot surface growth. With the addition of ammonia, the value of sp2/sp3 (indication of the graphitization degree of soot particles) did not change much for XNH3 from 0 to 0.17 then increased significantly, which indicated the degree of graphitization of soot particles significantly increased with ammonia addition. The intensity of the N1s peak (indication of the N-containing species in soot) increased with the addition of ammonia. This study confirmed that the addition of NH3 promotes the graphitization of soot.

Assessment of magnetic effects on soot characteristics in inverse diffusion ethylene flames

The magnetic effect on soot properties in ethylene inverse diffusion flames (IDF) was investigated in this study. The investigation involved the use of high-resolution transmission electron microscopy analysis (HRTEM), Raman spectroscopy analysis, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction spectroscopy (XRD) to examine the nanostructure and graphitization degree of soot collected from flame exhaust gas at various height above burner surface (HAB) under both magnetic and non-magnetic conditions. Increasing the magnetic flux density resulted in modifications to soot properties. When the sampling height was HAB = 4 cm, increasing magnetic flux density resulted in longer fringe lengths, lower fringe tortuosity, less amorphous carbon content and surface oxygen content for the collected soot from flame exhaust gas. These results indicated higher graphitization degrees, which may be attributed to longer residence time and oxidation of soot particle in flames. Moreover, when the sampling height increased from HAB = 4 cm to 6 cm under non-magnetic condition, the nanostructure of soot in the flame exhaust gas was more organized, possible due to the oxidation of soot at the region between HAB = 4 and 6 cm region. However, with the magnetic field on, the crystalline structure of soot in the flame exhaust gas became increasingly disordered as the sampling height increased. This suggested that the soot may also be affected by the magnetic effects in addition to oxidation at the region between HAB = 4 and 6 cm region. The magnetic effect could trigger the transformation of graphitic carbon to amorphous carbon in soot particles as they passed through the magnetic field. With more elaborated magnetic fields, the magnetic effect on soot could contribute to strategies controlling soot emissions and removal.

Effects of NH3 and H2 addition on morphology, nanostructure and oxidation of soot in n-decane diffusion flames

The effects of ammonia and hydrogen addition on soot formation characteristics in n-decane laminar diffusion flames were studied. The addition of argon was specifically considered to identify the chemical effect of ammonia. The flame temperature, particle morphology, and oxidation characteristics were analyzed. Results showed that both ammonia and hydrogen addition increase the flame height and suppress soot formation, while the suppression effect of ammonia is more pronounced. The addition of argon or ammonia reduces the temperature of flame upstream and yields the similar flame temperature, while hydrogen addition increases the flame temperature. Compared to the flame with argon, the addition of ammonia delays particle nucleation, indicating that the soot nucleation and growth process are chemically inhibited. In contrast, doping hydrogen leads to an earlier nucleation process and aggregation phenomenon. Further analysis on particle nanostructure indicated that the addition of ammonia yields shorter lattice fringes, larger interlayer spacings and amorphous carbon contents, demonstrating a looser and higher disorder internal structure. The addition of hydrogen yields longer fringes and smaller interlayer spacings, showing the particles have a more compact internal structure and higher degree of graphitization. This indicates hydrogen addition reduces the oxidation activity of the particles, which is confirmed by thermogravimetric analysis.

Characterization of soot emitted from the atmospheric combustion of diethyl ether-diesel blends

In accordance with the European commission’s renewable energy proposal for 2030, advanced biofuels should be blended at a minimum of 3.6 % with conventional fuels used for powering internal combustion engines. Ethers, which may be produced using modern production methods from sustainable sources like biomass, may be crucial in this regard in the future. This study demonstrates the impact of diethyl ether as a blend component (mixed with diesel) on the characteristics of the soot generated from the diethyl ether-atmospheric diesel's combustion. The soot used in this work came from a smoke point lamp that burned a mixture of diesel and diethyl ether as per ASTM D1322 standard. Diethyl ether (DEE) and diesel (D) were combined in the following blends: DEE5D (5 % diethyl ether and 95 % diesel v/v), and DEE20D (20 % diethyl ether and 80 % diesel v/v). The obtained soot was characterized in detail using the following: elemental analyzer, X-Ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), transmission electron microscopy (TEM), RAMAN spectroscopy, thermogravimetric analysis (TGA), and proton nuclear magnetic resonance (1H NMR) spectroscopy. According to the results from XRD and Raman spectroscopy, the soot nanostructure is influenced by the amount of diethyl ether present in the mixture, which raises the reactivity. The results of the elemental analyzer and 1H NMR matched those of the TGA's soot reactivity (oxidations). The results from the SEM and TEM tests, however, were not enoughto support the experimental findings.

Hydrogen, sp2 Carbon Hybridization, and sp2 Clustering as Pieces of the Puzzling Nanostructure of Soot: A Closer Look

Hydrogen, sp² Carbon Hybridization, and sp² Clustering as Pieces of the Puzzling Nanostructure of Soot: A Closer Look

Effect of NH3 addition on soot morphology and nanostructure evolution in laminar ethylene diffusion flame

Ammonia, as a carbon neutral alternative fuel, has attracted wide attention. However, due to the defects in the combustion performance of pure ammonia, it is still necessary to further solve this problem in practical utilization. The purpose of this paper is to study the influence of ammonia on the morphology of soot and the evolution of nanoparticle structure in laminar flame of ethylene. In this work, the soot collected by thermophoresis probe was observed by the high resolution transmission electron microscope (HRTEM), and the image information in HRTEM images was statistically processed, and the graphitization degree of soot was measured by X-ray diffraction (XRD) spectrum of soot samples. The experimental results show that the addition of ammonia can inhibit the growth of soot nuclei and delay the formation of incipient soot, and has different effects on the evolution of soot morphology and structure in ethylene flame. It is noteworthy that the soot samples collected in the upstream part of the ammonia-doped flame show more mature core–shell structure in HRTEM images and more graphitized XRD diffraction data than those collected in pure ethylene flame. The main reason may be the chemical effect of ammonia and the thermal effect caused by the reduction of flame radiation loss, which have different effects on the nanostructure and morphology of soot at different stages of soot formation. Fringe structure model is used to describe and explain the influence of soot in flame with height before and after ammonia doped.

Characterization of soot emissions formed in a compression ignition engine cofired by ammonia and diesel

The impact of ammonia (NH3) co-firing with diesel on the greenhouse gases (GHG) and soot emissions of compression ignition (CI) engines is a current concern in large-scale agriculture, marine transportation and shipping applications for which NH3 is proposed as a near-term decarbonization solution. In this study, the effect of NH3 port injection on the GHG emissions and the characteristics of the soot formed in a NH3-diesel dual fuel CI engine is investigated. Soot is sampled from the engine exhaust operating in dual-fuel mode at 20% and 40% NH3 energy fraction and in diesel-only mode at a fixed engine speed, load, and diesel injection strategy. Detailed analysis of soot is done to investigate: the exhaust soot yield using gravimetric analysis, soot growth and inception through the average primary particles size and number concentration using analysis of Transmission Electron Microscopy (TEM) imaging, the soot nanostructure using Raman spectroscopy, and the chemical composition using X-ray Photoelectron Spectroscopy (XPS). The engine GHG emissions measurements shows that carbon dioxide (CO2) is reduced while N2O emissions increases with NH3 addition. The engine soot emissions yield is significantly reduced with the average primary particles size and number concentration decreasing as the NH3 energy fraction increases. The soot nanostructure is impacted by NH3 addition as it becomes more graphitic with high ratio of sp2 to sp3 carbon bonding. The XPS chemical composition analysis also shows an increase in the nitrogen bonding with carbon in the aromatic rings on the particles surface. The results suggest that the chemical interaction of NH3 with diesel results in soot with more graphitic nanostructure as nitrogen reaction with carbon at active defect sites leads to an increase in the nitrogen content on the soot surface with NH3 addition. This indicates an increased potential of NH3 co-firing with diesel to form nitrogenated PAHs (N-PAH) on the soot surface which would require further studies to identify the risks posed on the environment and human health.

Insight of soot nanostructure and oxidation behavior in ammonia / ethylene coaxial diffusion flame

In this work, the effects of ammonia addition on the morphology evolution, nanostructure and oxidation reactivity of soot particles in ethylene laminar diffusion flame were investigated. Soot sampling was performed using a thermophoresis probe and the morphological evolution of the particles was observed by transmission electron microscopy. In addition, high resolution transmission electron microscopy, Raman spectroscopy and thermogravimetric analysis were adopted to study the nanostructure and oxidation reactivity of soot particles sampled by quartz plate samples. The experimental results show that ammonia addition increases the flame height and compresses the soot formation region, delaying the evolution of each generation stage. For the primary soot particles, the surface growth is inhibited by ammonia doping, and the average particle size d¯p is reduced by about 33.13%. In addition, ammonia doping greatly inhibits the condensation between the primary particles of soot, and the parameters of the agglomerates such as the average area of the agglomerates A¯a, the number of primary particles N¯p and the fractal dimension Df are greatly reduced. Compared to the 100% argon doping ratio, ammonia doping reduced the average area of the agglomerates by approximately 76.27%, and the number of primary particles contained in the aggregate decreased by about 50%. The fringe length of soot particles decreases by about 15.38%, the fringe spacing increases by about 1.67% and the fringe tortuosity increases by about 4.23%, indicating that the degree of graphitization of soot decreases, the nanostructure becomes more disordered and the possibility of soot oxidation increases. The addition of ammonia results in the increase of disordered carbon in the soot of ethylene flame, and the activation energy of soot decreases significantly, so the soot has stronger oxidation reactivity.

Quantification of soot nanostructure produced from a diesel engine fueled with C3 ketone

The soot emission is an urgent problem that deserves extensive studies to suppress it. The smallest ketone was investigated in this study as a soot suppressor in a diesel engine. The fringe analysis approach was used to quantify the nanostructure characteristics of soot. At first, the image processing parameters were updated for this study, and their effects were explored and interpreted. Image resolution was found to be a crucial parameter in the image analysis process with a spatial resolution of 0.0417 nm/pixel as the best adjustment for the present study. The contrast-limited adaptive histogram equalization approach provided a perfect histogram equalization. A Gaussian low-pass filter with a standard deviation of 1.5 and a filter size of 11 produced the best results. The bottom hat transformation with a structuring element of a five pixels size and zero corners produced the best fringes' representation. A threshold level of 0.8 as Otsu's level provided a better nanostructure's representation. Second, the images of soot from acetone/diesel blends were analyzed using the updated parameters. The addition of acetone reduced the formation of soot in a diesel engine. The fringe length, tortuosity, intensity and alignment were all decreased, while fringe spacing was increased with acetone.

Experimental Study of Oxygen Depletion Effects on Soot Morphology and Nanostructure in Coflow Diffusion Aviation Fuel (RP-3) Flames

Oxygen concentration is a significant factor affecting soot formation and oxidation. However, there are few studies that have focused on the morphology and nanostructure characteristics of soot in aviation kerosene, oxygen-depleted combustion flames. In the present paper, five coflow flames under initial oxygen volume concentrations of 18.5%, 19%, 20%, 21%, and 23.5% were studied. The pneumatic probe sampling method and high-resolution transmission electron microscopy (HRTEM) analysis were conducted to quantify the morphology and nanostructure parameters, and laser extinction (LE) was applied to determine the soot volume fraction. Among the cases of different oxidizer oxygen concentrations (23.5% to 18.5%), the change in soot volume fraction was quantified, and the degree of graphitization of soot particles, i.e., the maturity, were compared. The results show that the peak value of soot volume fraction of the flames increased by 0.73 ppm as the oxygen concentration increased from 21% to 23.5%, and decreased by 1.25 ppm as the oxygen concentration decreased from 21% to 18.5%. When the oxygen concentration decreased from 23.5% to 18.5%, the soot primary particle diameter at the same dimensionless height decreased and then increased, which was attributed to the competition between the changes in the residence time and the growth rate of the soot particles. The quantitative analysis results of the soot nanostructure suggested that reduced oxygen concentration inhibited the graphitization process of carbon lattices and decreased the maturity and oxidation resistance of soot. When the oxygen concentration decreased from 23.5% to 18.5% at the same dimensionless height, the mean fringe length decreased by an average of 0.18 nm, and the mean value of fringe tortuosity and spacing increased by an average of 0.053 and 0.035 nm.

The effect of ammonia addition on soot nanostructure and composition in ethylene laminar flames

The formation of soot in ammonia (NH3) combustion with a hydrocarbon such as ethylene (C2H4) is investigated using the analysis of particles’ nanostructure and surface chemical composition to identify the mechanisms by which NH3 suppresses soot growth. Young and mature soot particles were extracted from laminar diffusion co-flow flames of NH3C2H4 blends up to 50% NH3. The soot nanostructure is examined using lattice fringe analysis of high-resolution transmission electron microscopy (HRTEM) images, Raman Spectroscopy, and Electron Energy Loss Spectroscopy (EELS). The chemical composition of the soot surface is analyzed using X-ray Photoelectron Spectroscopy (XPS). With increasing NH3 addition, reduced planar growth of the soot graphitic layers is observed through the analysis of the soot nanostructure which indicates the suppression of carbon addition at the edge sites of the layer planes. It is also found that the carbon sp2/sp3 bonding ratio increases which shows a nanostructure with less carbon sp3 bonding at defect sites. By exploring the chemical composition, the nitrogen content of the soot surface increases with NH3 addition which is caused by the bonding of nitrogenated species with carbon at defect and edge sites of the carbon layer, reducing the potential for carbon addition, and thus soot growth. The results also show an increased risk of formation of nitrogenated polyaromatic hydrocarbons (N-PAHs) on the soot surface by NH3 addition. The study presents a novel investigation of the impact of NH3 on the soot surface chemistry and particles nanostructure which explains the role of NH3 in suppressing soot growth and reveals the potential for new toxic characteristics for the soot emissions formed in NH3-hydrocarbon cofired systems.

Effect of Potassium Chloride on the Nanostructure and Reactivity of Soot Particles from Combustion of Municipal Solid Waste

This work studied the effect of potassium chloride (KCl) on soot formation during the combustion of municipal solid waste (MSW). The nanostructural and oxidative properties of soot particles were characterized by high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) spectroscopy, Raman spectroscopy (RS), and thermogravimetric analysis (TGA). HRTEM images showed that, under the same combustion environment, the KCl-loaded fuel samples generated soot particles with smaller particle sizes and more compact morphologies. Quantification of the nanostructure further indicated that, with increasing potassium concentrations from 1 to 5%, the fringe separation distance and fringe tortuosity of soot particles slightly increased, yet no clear trend was observed in the fringe length. Raman spectral analysis verified the fringe analysis, suggesting that the addition of KCl made the soot nanostructure more disordered with a larger separation distance and higher fringe tortuosity. In addition, oxidation profiles determined that the reactivity of K-doped soot was enhanced because of a decrease in the apparent activation energy (Ea) from 167 to 124 kJ/mol. Moreover, Ea showed strong linearity with the fringe tortuosity and fringe separation distance, with R2 values of 0.91 and 0.97, respectively. On the basis of the experimental data, a schematic of four K–soot interaction routes is proposed to better understand the soot formation during the combustion of solid wastes.

Effects of ammonia on morphological characteristics and nanostructure of soot in the combustion of diesel surrogate fuels

The morphological characteristics and nanostructure of soot particles in pure n-heptane (C7H16) and n-heptane/ammonia co-flow diffusion flames were analyzed and compared using thermophoretic sampling and transmission electron microscopy (TEM) observation combining with quantitative image information extraction methods. The results showed that the overall formation and evolution of soot particles in NH3-doped n-heptane flames along the flame centerline were similar with that without NH3-doping. However, compared to n-heptane flame, the peak average diameter of primary soot particles and the peak gyration radius of soot aggregates in NH3-doped flames were reduced by about 45% and 37%, respectively, which indicated that the growth of both primary soot particles via surface reaction/condensation and soot aggregates via coagulation were significantly decreased. Meanwhile, the fractal dimension of soot aggregates was lower with NH3 addition as the structure of soot aggregates was looser and tended to be more chain-like. After NH3 doping, the peak average fringe length inside soot particles was decreased by 13%, and the inter-fringe spacing and tortuosity of soot were increased by 8% and 3%, respectively. This represented a more disordered microcrystal structure and lower degree of graphitization of soot particles, meaningfully indicating a higher oxidation reactivity.

Effects of ammonia addition on soot formation in ethylene laminar diffusion flames. Part 3. The morphology and nanostructure of soot particles

Ammonia (NH3) fuel has been widely considered a competitive alternative fuel and hydrogen carrier due to its “non-carbon and hydrogen-rich” nature. In this study, the thermophoretic sampling combined with transmission electron microscopy (TEM) analysis was conducted to investigate the effects of NH3 addition with varying ratios (between 0% and 60% by volume fraction while the remainder is argon) on the evolution of morphology and nanostructures of soot particles along the flame axis in the ethylene (40% by volume fraction) co-flow diffusion flames. Results showed that the flame visible height increased with the addition of NH3, and the flame temperature decreased at the height above burner (HAB) below 30 mm while increased at HAB > 30 mm. With NH3 addition, the size of soot (primary particles and aggregates) and the number of soot primary particles contained in the soot aggregates decreased significantly. In addition, the investigation of soot nanostructures showed that the carbon layers with shorter fringe length (Fl) and higher tortuosity (Ft) would be oxidized before it arrived to the flame tip in the NH3-doped flame, resulting in the longer Fl and higher Ft. In general, the inter-fringe spacing (Fd) increased with NH3 addition. The evolution of soot morphology and nanostructures indicated that NH3 would delay the process of particle inception and surface growth.

Strongly reduced optical absorption efficiency of soot with addition of potassium chloride in sooting premixed flames

Optical properties of soot have been investigated with and without potassium chloride (KCl) salt added to the soot formation process in a premixed ethylene/air flame. A strong decrease in optical absorption efficiency of the soot was observed with increasing amounts of KCl added to the fuel based on the method of fluence curve analysis using laser-induced incandescence (LII). To understand the reason for this major change in absorption efficiency, probe sampling and subsequent structural analysis were performed using Raman spectroscopy and high-resolution transmission electron microscopy (HRTEM). Raman spectra indicated no significant difference between the nanostructure of soot from the two main cases; a reference case without addition of salt, and a case with addition of ∼600 ppm K. In the case of K addition, HRTEM showed slightly less compact nanostructure signified by somewhat shorter interlayer spacing, and significantly different polar ordering of carbon lamellae indicating smaller primary particles, thereby supporting previous TEM studies on soot sampled from the same flames showing smaller soot particle sizes with KCl addition. The impact on soot absorption properties from the observed differences is discussed. It is speculated that the main cause for the lower absorption with K addition is a quantum confinement effect due to reduction in soot particle size.