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1.
A method of long-lasting TiO2 nanoparticle generation was tested for use in follow-up studies of the health impacts of nanoparticles on laboratory animals during several weeks' long exposure experiments. Nanoparticles were synthesized in an externally heated tube reactor by pyrolysis and oxidation of titanium tetraisopropoxide. Particle production was studied under varying reactor temperature, reactor flow rate, and precursor vapor pressure. A total of 264 h of particle generation were performed in four experimental campaigns using one batch of precursor without an observable decrease of particle production. As a result, particle production with number concentrations high above 1.0 × 107 #/cm3 and with primary particle sizes well below 50 nm could be achieved in most of the investigated experimental conditions. Maximum of particle mass concentration reached the value 9500 μg/m3, which corresponds with emission rate 29 μg/min. The dependence of nanoparticle production and characteristics on experimental conditions was evaluated and the most suitable parameters for exposure experiments were specified. A comparison of the results with data from the literature shows that the material of the reactor plays a significant role in the process of particle formation.

Copyright © 2016 American Association for Aerosol Research  相似文献   


2.
Thin films of controlled morphology were fabricated by electrospray drying a colloidal nanoparticle suspension using a conductive and volatile solvent and impacting the nanoparticles on a substrate. Three parameters were used for control: impact velocity, size of the nanoparticles or nanoparticle agglomerates, and solvent volatility. The impact velocity was controlled by charging nanoparticles through electrospray dispersion and varying the electric field driving the particle impaction. It was found that the structure is governed by the relative importance of charged particle drift imposed by the external electric field and the thermal velocity due to Brownian motion. Peclet number correlates with the morphology of the deposit where columnar structures result from high Pe, corresponding to ballistic deposition and porous, fractal-like structures result from small Pe. These patterns match predictions based on Monte Carlo simulations in the literature. For dispersions with higher nanoparticle concentrations, droplet evaporation causes densification of the particle ensemble to form a spherical aggregate that deposits in a predominantly ballistic manner, with smaller aggregates forming denser films. If the droplet evaporation lifetime is altered for the aggregates to be partially wet upon impacting the substrate, the subsequent rapid evaporation of the remaining solvent on the substrate leads to formation of films with high interconnectivity. Films formed by the electrospray technique have large-scale uniformity and their structure is independent of thickness. The interpretation of the observed morphologies in terms of Peclet number and Damkhöler number provides a conceptual framework for a rational design of film structures as required by many applications.

Copyright © 2017 American Association for Aerosol Research  相似文献   


3.
There exists a demand for production of metal nanoparticles for today's emerging nanotechnology. Aerosol-generated metal nanoparticles can oxidize during particle formation due to impurities in the carrier gas. One method to produce unoxidized metal nanoparticles is to first generate metal oxides and then reduce them during sintering. Here, we propose to instead prevent oxidation by introducing the reducing agent already at particle formation. We show that by mixing 5% hydrogen into the nitrogen carrier gas, we can generate single crystalline metal nanoparticles by spark discharge from gold, cobalt, bismuth, and tin electrodes. The non-noble nanoparticles exhibit signs of surface oxidation likely formed post-deposition when exposed to air. Nanoparticles generated without hydrogen are found to be primarily polycrystalline and oxidized. To demonstrate the advantages of supplying the reducing agent at generation, we compare to nanoparticles that are generated in nitrogen and sintered in a hydrogen mixture. For bismuth and tin, the crystal quality of the particles after sintering is considerably higher when hydrogen is introduced at particle generation compared to at sintering, whereas for cobalt it is equally effective to only add hydrogen at sintering. We propose that hydrogen present at particle generation prevents the formation of oxide primary particles, thus improving the ability to sinter the nanoparticles to compact and single crystals of metal. This method is general and can be applied to other aerosol generation systems, to improve the generation of size-controlled nanoparticles of non-noble metals with a suitable reducing agent.

Copyright © 2018 American Association for Aerosol Research  相似文献   


4.
The increasing need for engineered alloy nanoparticles (NPs) in diverse fields has spurred efforts to explore efficient/green synthesis methods. In this respect, spark ablation provides a scalable and viable way for producing widely different types of mixed NPs. Most importantly, implementation of the spark has the great advantage to combine a wider range of materials, thereby allowing the synthesis of mixed NPs with virtually unlimited combinations. Here we show that polarity reversal of spark discharges between two electrodes consisting of different materials enables synthesis of alloy NPs, while having a good potential to control the broadness of their composition distribution. A model developed in this work provides a tool for tuning the ablation ratio between the electrodes by adjusting the electric characteristics of the spark circuit. The ablation ratio is equal to the mean composition of the resulting NPs. The model predictions are in accordance with measurements obtained here and in earlier works. The unique way of producing alloy NPs by spark ablation shown in this work becomes especially useful when the starting electrode materials are immiscible at macroscopic scale.

Copyright © 2018 American Association for Aerosol Research  相似文献   


5.
Sampling and dilution of flame-generated, fractal-like ZrO2 aerosols is investigated by aerosol mass/mobility measurements and microscopy. Two broadly used sampler configurations, a straight-tube (ST) and a hole-in-a-tube (HiaT), at three different in-flow orientations and hole diameters are evaluated. The mobility size distributions, mass-mobility exponent, Dfm, prefactor, kfm, and average primary particle diameter are obtained at 10–60 cm height above the burner (HAB) of fuel-rich (hot) and fuel-lean (cold) spray flames by differential mobility analyzer (DMA) and aerosol particle mass (APM) measurements using a recent power law for fractal-like particles. The primary particle diameter, agglomerate size distributions, and corresponding standard deviations from aerosol measurements are compared to those by counting images of particles collected by thermophoretic sampling along the flame centerline. Once new particle formation is completed in the flame, both sampler configurations result in nearly identical particle size distributions. Furthermore, all HiaT samplers result in similar mobility size distributions at all orientations, regardless of hole size. Sampling using a downstream in-flow hole orientation results in slightly larger Sauter mean diameters than those obtained by upstream or sidestream ones, especially for the cold flame. Additionally, a correlation is developed by Discrete Element Modeling (DEM) for the agglomerate Dfm evolution to its asymptotic value of 2.2 as function of the average number of primary particles per agglomerate, nva, or the relative particle density with pre-exponential constant kfm = 1.18, regardless of primary particle size. This is in good agreement with an experimentally obtained correlation in terms of relative particle density as well as with experimental data for ZrO2, Ag, and Cu nanoparticles.

© 2016 American Association for Aerosol Research  相似文献   


6.
Spectrophotometric methods developed previously to quantify the major functional groups present in oxidized organic aerosol were modified for use with sample masses typical of those collected from ambient air. In these methods, carbonyl, hydroxyl, carboxyl, and ester groups are reacted with derivatizing agents that are specific to each functional group to form strongly light absorbing derivatives, a colored peroxide solution is formed through redox chemistry, and nitrates have an inherently strong absorbance. As described here, improved detection limits are made possible by measuring absorbance using a spectrophotometer that requires only a few microliters of solution for analysis, instead of the five milliliter volume required previously when using a standard cuvette. Use of this so-called NanoPhotometer allows comparable absorbances to be obtained with much less mass by concentrating samples by more than two orders of magnitude relative to previous methods. Detection limits are approximately 0.03, 0.02, 0.3, 1, 1, and 0.07 nmoles for carbonyl, hydroxyl, carboxyl, ester, peroxide, and nitrate groups, which correspond to approximately 0.8, 0.6, 10, 40, 50, and 5 ng of each functional group. In practice, depending on the composition of functional groups, the mass required for complete analysis of moderately oxidized organic aerosol is ~10–100 µg. The new microscale methods were shown to provide good linearity, precision, and accuracy by comparing results from the analysis of standards and aerosol formed from reaction of α-pinene and O3 with results obtained using the previously developed macroscale methods. The evaluation demonstrates that the microscale methods can be used to quantify these six functional groups at low organic aerosol mass concentrations.

Copyright © 2016 American Association for Aerosol Research  相似文献   


7.
Composite nanoparticles find application in catalysis, drug delivery, and energy storage and require increasingly fine control of their physical properties and composition. While composite nanoparticles have been widely synthesized and characterized, little work has systematically correlated the initial concentration of precursors and the final composition of flame synthesized composite nanoparticles. This relationship is explored in a diffusion flame aerosol reactor by coupling a scanning mobility particle sizer (SMPS) with an inductively coupled plasma optical emission spectrometer (ICP-OES). A framework for studying the relationship between the initial precursor concentrations of different elements and the final nanoparticle composition is explored. The size-resolved elemental composition was measured by directly injecting size-selected fractions of aggregated magnetite and silicon dioxide composite nanoparticles into the ICP-OES plasma. This work showed a correlation between precursor molar ratio and the measured elemental ratio in the mobility size range of 50 to 140 nm. Building on previous work studying size resolved elemental composition of engineered nanoparticles, the analysis is extended to flame synthesized composite nanoparticle aggregates in this work.

Copyright © 2017 American Association for Aerosol Research  相似文献   


8.
An experimental method is developed for the purpose of simulating plutonium aerosol source terms with conventional metals in laboratory. In this method, metal samples are aerosolized by high explosive detonation in a containment vessel. Aerosols having aerodynamic diameter (AD) less than 10 µm are then collected by a cascade impactor and analyzed by atomic absorption spectroscopy. Two sets of experiments were conducted. In the first set, five candidate metal samples (Ag, W, Sn, Ce, and V) were tested. It is found that the cumulative mass distribution of silver under certain conditions was in good agreement with that of plutonium from the Operation Roller Coaster-Double Track experiment. Thus, silver is chosen as a surrogate to simulate the plutonium aerosol source term. In the second set, silver aerosol source term was studied in detail with different test configurations. The results demonstrate that the peak of the mass-size distribution of silver is in the AD range 1.1–3.3 µm. The amount and fraction of relatively small silver aerosols decrease significantly with time due to coagulation and deposition. Interestingly, the amount of silver in aerosols could be expressed as a quadratic function of the peak detonation pressure.

© 2016 American Association for Aerosol Research  相似文献   


9.
This article introduces an aerosol-based technique to make aqueous suspension of hydrophobic nanomaterial without adding dispersant. The method is intended for making a test-sample for evaluating the toxicities of nanomaterial by intra-tracheal administration. The method can wet the surface of hydrophobic nanomaterial within a few seconds. After the wetting process five to ten minutes of sonication assisted with manual stirring can fully disperse the hydrophobic nanomaterials in water. Two types of TiO2 nanomaterial were used in this study; Tayca JMT-150IB whose surfaces are coated with negatively charged hydrophobic functional group, and P25 whose surfaces are naturally hydrophilic. Nanomaterials are aerosolized by a dry-method and become micrometer-sized agglomerates. Then supersaturated water vapor is condensed onto these airborne agglomerates by using a growth tube collector. The collected suspension (CS) of hydrophobic nanomaterial (JMT-150IB) is prepared in two steps; airborne agglomerates are collected onto a flat surface then transferred to liquid-water and subsequently sonicated for complete dispersion. This method works equally well for making the CS of hydrophilic nanomaterial. Size distribution measurements of the CS show that airborne agglomerates of TiO2 dissociate into smaller units of agglomerates once they are captured into water, and the sizes of the agglomerates are in the nanometer to sub-micrometer range. Light scattering technique is used to show that a short sonication process can reproduce the particle number concentration of the CS after long storage.

Copyright © 2017 American Association for Aerosol Research  相似文献   


10.
Abstract

Laser derivatization is proposed as a diagnostic technique toward identifying the sources contributing to combustion produced soot. Fuel chemistry and the resultant oxygen content in nascent soot have been shown to influence the evolution of soot nanostructure upon laser derivatization. This is illustrated using the spectroscopic and microscopic characterization of biodiesel soot, with a systematic variation in fuel chemistry used to generate the soot. Functionalized carbon black is used as the control to independently verify the influence of material chemistry on nanostructure upon laser heat treatment. Results track with those observed for biodiesel soot. Reciprocally, the similarity in soot nanostructure observed after laser heating is tied to the likeness in fuel chemistry of biomass-fueled sources. Understanding the origin of differences or similarities in soot nanostructure upon laser heat treatment can help differentiate sources based on their contribution, thereby aiding in effective air quality control.

Copyright © 2019 American Association for Aerosol Research  相似文献   

11.
Dielectric barrier discharge (DBD) and spark discharge, two versatile atmospheric pressure plasma-based techniques, have been employed to generate nanoparticles. This study compares the characteristics of metal nanoparticles generated by a DBD reactor and a spark discharge generator with argon as the working gas. The gas temperature in the discharge region of the DBD reactor remained near room temperature, while that of the spark reactor varied from 470 to 1120 K and generally increased with increasing applied voltage amplitude in the range of 2–10 kV and driving frequency in the range of 1–10 kHz. Comparing to spark-generated nanoparticles under the same voltage, frequency, and flow rate, DBD-generated nanoparticles have smaller sizes, better monodispersity, and lower number concentrations. The number concentration of DBD-generated particles decreases significantly under high working voltage and frequency, while the number concentration of spark-generated particles increases with increasing working voltage. Under continuous operations over several hours, the DBD reactor has better temporal stability in generating nanoparticles than the spark generator.

© 2017 American Association for Aerosol Research  相似文献   


12.
Resuspension is considered as a source of indoor air pollutants. These airborne pollutants can be in the form of liquid or solid. It has been previously found that the detachment mechanism of liquid droplets is different from the solid particles on the poly(methyl methacrylate) (PMMA) surface. Liquid droplets detach by portion when they are under an increasing normal force field while droplets detach completely when under a tangential force field. In this research, droplet detachment experiments are extended to different substrate materials, which are PMMA, glass, and stainless steel by the means of centrifuge. Also, the differences in detachment between pure glycerol-water (pure fluid) and a glycerol solution with the addition of nanoparticles (nanofluid) are investigated under different substrate materials. It is found that liquid droplets, again, detach by portion under normal force for all the substrate materials. For tangential force, the droplets detach completely if the exerted force was sufficiently large and the threshold values are material dependent, which is further elaborated by retention theory. After the addition of nanoparticles, a higher removal force was required compared to the droplets of pure fluid within the same size range. Also, solid residues with a negligible amount of fluid were found on the substrate after each removal of droplets under both normal and tangential force. The involvement of nanoparticles could be the pioneer work for future studies on commonly found liquid pollutants, which are prone to be contaminated by solid particles, such as in salivary excretion.

Copyright © 2018 American Association for Aerosol Research  相似文献   


13.
Few studies reported the formation of Ti-containing clusters in the initial stages of TiO2 flame synthesis. The conversion from synthesis precursor to TiO2 monomers was commonly assumed to take place through global reaction such as thermal decomposition and/or hydrolysis at high temperatures. More recent studies have been able to identify stable intermediates of Ti-containing monomers, most commonly Ti(OH)4, as the final step before the formation of TiO2. However, no larger Ti-containing cluster formation mechanisms or interactions between these monomers have been tracked. To investigate cluster formation pathways of TiO2 during flame synthesis, Charged clusters were measured in an atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometer. TiO2 nanoparticles were synthesized by adding titanium tetraisopropoxide (TTIP) precursor to a premixed CH4/O2/N2 flat flame aerosol reactor. Pure TiO2 clusters were not detected by the APi-TOF. Results from measured mass spectra and mass defect plots show that for positively charged clusters, the abstraction of CH2 groups occurs simultaneously with the clustering of larger intermediate organometallic species. For negatively charged clusters, NOx formation pathways in the flame may play a role during the initial stages of TiO2 formation, since a lot of Ti-containing clusters were attached with nitrate-related species. These research findings provide insights on quantum dot synthesis and molecular doping where rapid dilution of the flame synthesized nanoparticles is needed to better control the particle size and chemical composition. The possible influences of and potential artifacts brought by the dilution system on observing the incipient particle formation in flames were also discussed.

© 2017 American Association for Aerosol Research  相似文献   


14.
The aim of this study is to investigate the effect nanosilica and nanoalumina has on nanoparticle release from industrial nanocomposites due to drilling for hazard reduction whilst simultaneously obtaining the necessary mechanical performance. This study is therefore specifically designed such that all background noise is eliminated in the measurements range of 0.01 particles/cm3 and ±10% at 106 particles/cm3. The impact nano-sized SiO2 and Al2O3 reinforced polyester has on nanoparticle aerosols generated due to drilling is investigated. Real-time measurement was conducted within a specially designed controlled test chamber using a condensation particle counter (CPC) and a scanning mobility particle sizer spectrometer (SMPS). The results show that the polyester nanocomposite samples displayed statistically significant differences and an increase in nanoparticle number concentration by up to 228% compared to virgin polyester. It is shown that the nanofillers adhered to the polyester matrix showing a higher concentration of larger particles released (between 20 – 100 nm). The increase in nanoparticle reinforcement weight concentration and resulting nanoparticle release vary considerably between the nanosilica and nanoalumina samples due to the nanofillers presence. This study indicates a future opportunity to safer by design strategy that reduces number of particles released concentration and sizes without compromising desired mechanical properties for engineered polymers and composites.

© 2017 American Association for Aerosol Research  相似文献   


15.
We have established a novel route for the synthesis of N-doped TiO2 by adopting flame aerosol (FSP) technique and investigated the effect of water content on the physico-chemical properties of the as-synthesized nanoparticles. The key characteristics of the developed method are to modify the precursor solution in order to incorporate nitrogen atoms into the TiO2 lattice without altering the FSP set-up. The reduction of the flame enthalpy resulting in N-incorporation into the TiO2 and the N-doping can be greatly enhanced further by the addition of secondary N-source (urea). Our XRD results reveal a shift of the (101) plane anatase diffraction peak to lower angles in our N-doped TiO2 compared to undoped TiO2, which suggest the distortion and strain in the crystal lattice prompted by the incorporation of the nitrogen atoms. The growth or expansion of crystal lattice can be attributed to the larger atomic radius of respective nitrogen atoms (r?=?1.7 Å) compared to oxygen (r?=?1.40 Å). Our XPS and EDX spectroscopy results elucidate that the nitrogen was effectively doped into the crystal lattice of TiO2 in our as-synthesized N-TiO2 catalysts predominantly in the form of interstitial nitrogen (Ti?O?N). The nitrogen atoms incorporation into the crystal lattice of titania modifies the electronic band structure of TiO2, resulting in a new mid-gap energy state N 2p band formed above O 2p valence band. This occurrence narrows the band gap of TiO2 (from 3.12 to ~2.51?eV) in our N-doped TiO2 and shifts the optical absorption to the visible region.

Copyright © 2018 American Association for Aerosol Research  相似文献   

16.
The ability to properly scale the synthesis of advanced materials through combustion synthesis routes is limited by our lack of knowledge regarding the initial stages of particle formation. In flame aerosol reactors, the high temperatures, fast reaction rates, and flame chemistry can all play a critical role in determining the properties of the resulting nanomaterials. In particular, multicomponent systems pose a unique challenge as most studies rely on empirical approaches toward designing advanced composite materials. The lack of predictive capabilities can be attributed to a lack of data on particle inception and growth below 2 nm. Measurements for the initial stages of particle formation during the combustion synthesis of SiO2 and composite SiO2/TiO2 using an atmospheric pressure inlet time-of-flight mass spectrometer are presented. Both positively and negatively charged clusters can be measured and results show the presence of silicic acid species which grow through dehydration, hydrogen abstraction, and interactions with hydroxyl radicals. In the case of composite SiO2/TiO2 particle formation, new molecular species containing Ti atoms emerge. Tandem differential mobility analysis-mass spectrometry (DMA-MS) provided further insight into the size-resolved chemistry of particle formation to reveal that at each cluster size, further hydroxyl-driven reactions take place. From this we can conclude that previous assumptions on collisional growth from simple monomer species of SiO2 and TiO2 do not sufficiently describe the collisional growth mechanisms for particle growth below 2 nm.

Copyright © 2018 American Association for Aerosol Research  相似文献   


17.
Abstract

For the purpose of silica surface layer modulation, a pneumatic-controlled two-substance atomizer with inertia-based coarse droplet separation was operated at different system pressures for tetraethyl orthosilicate precursor aerosol supply during combustion chemical vapor deposition. A comprehensive testing study was performed to characterize the atomizer’s performance characteristics, initial precursor aerosols at the atomizer’s outlet, transformed aerosols before combustion, combustion aerosols and formed layers. Laser diffraction spectrometry, differential electrical mobility analyses and condensation particle counting were used for aerosol characterization with regard to particle size and particle production quantities. Layers were characterized by scanning electron microscopy, atomic force microscopy, spectral ellipsometry, water contact angle measurements and light transmission concerning geometric properties (thickness, surface structure and roughness) and physical behaviors (i.e., optical behaviors, hydrophobicity). Results show a quasi-linear relationship of the ejection mass flow of the pneumatic-controlled atomizer and geometric layer properties which again show a direct relationship to the physical properties. No correlation was found between the aerosols before combustion and the combustion aerosols since the majority of combustion aerosol particles are synthesized solely from the gas phase based on evaporated precursor material.

Copyright © 2020 American Association for Aerosol Research  相似文献   

18.
Allothermal cracking of methane is a suitable and eco-friendly way to simultaneously produce hydrogen and carbon black. The economic viability of the process relies on the ability to produce carbon black having well-defined characteristics, particularly concerning the particle size. A model for the study of the carbon particle size distribution during thermal cracking of methane has been developed. The model takes into account: heat transfer by conduction, convection, particle and gas radiation, homogenous and heterogenous reactions of methane dissociation, nucleation, and growth of solid carbon particle formed. The model alleges nanoparticles are in thermal equilibrium and do not impact the flow. A parametric study is made on operating pressure and temperature. As a result, the increase of the pressure and temperature increases the yield of thermal methane cracking. Moreover, results show a particle size distribution becoming narrower with increasing temperature and/or pressure. In these conditions, the particles population tends to be monodispersed.

Copyright © 2016 American Association for Aerosol Research  相似文献   


19.
Past studies have shown that the diffusion-limited cluster aggregation mechanism yields aggregates with a mass fractal dimension (Df) of around 1.8 and power-law prefactor (kf) ranging between 1.2 and 2.5. For a fixed Df, an increasing kf physically manifests as decreasing shape anisotropy or the degree of “stringiness” of an aggregate. In this work, we investigate the effects of changing kf, monomer size (d), and number of monomers (N) of computer-simulated aggregates on their mass-mobility scaling exponent (Dfm) and prefactor (kfm). Our simulation results for a statistically significant number of Df = 1.78 ± 0.10 aggregates yielded Dfm values of 2.20 ± 0.05. These values are in excellent agreement with previous experimental observations. While variations in Dfm were predominantly influenced by Df, kfm showed sensitivity to fluctuations in kf. The validity and accuracy of the empirical power-law exponent 1.08 used for estimating N in three dimensions from two dimensional projection images was also evaluated. It was found that the exponent was only valid for aggregates with kf close to unity. A correction has been proposed to account for the enhanced apparent screening effects at large kf.

© 2016 American Association for Aerosol Research  相似文献   


20.
Metal screens with uniform micrometer-sized opening were employed to sieve aerosol particles by suppressing the adhesion of particles smaller than the openings. The collection efficiencies of monodispersed polystyrene latex (PSL) particles were experimentally determined using the metal screens with 1.2, 1.8, 2.5, and 4.2 μm openings at various filtration velocities. The particles smaller than the mesh opening adhered on the metal screen at a low filtration velocity, but the bounce-off of particles on the mesh surface suppressed the adhesion at a high velocity. As a result, we found that the adhesion of PSL particles larger than 0.3 μm mostly suppressed at a filtration velocity higher than 10 m s?1 and therefore we can sieve aerosol particles according to the opening size of metal screens. We also found that the particle number concentration could be determined by measuring the increase in pressure drop since the clogging of metal screen openings takes place by the individual particles.

© 2016 American Association for Aerosol Research  相似文献   

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