Role of oleic acid coating in the heterogeneous uptake of dimethylamine by ammonium sulfate particles

Reactive uptake by ammonium (NH₄⁺) salts is one of the major pathways for the gas-to-particle partitioning of alkyl amines. Recent studies using particles of individual ammonium salts and mixtures with hydrophilic organics have revealed that the degree of amine uptake depends on the phase state of ammonium salts, the particulate water contents and particle viscosity. The role of hydrophobic organic compounds, another important category of particulate organics commonly detected in the ambient atmosphere, in amine uptake remains unknown. Here we report the uptake of dimethylamine (DMA) by ammonium sulfate (AS) particles coated with fresh or ozone-aged bulk oleic acid (OA) at 60%, 30%, and <5% relative humidities (RHs) using an electrodynamic balance coupled with Raman spectroscopy. OA and DMA were selected to represent hydrophobic organics and alkyl amines, respectively. Over 74% of the original NH₄⁺ ions were displaced due to DMA uptake, except those conditioned at <5% RH. On the other hand, the fresh or aged bulk OA coating retarded DMA uptake by preventing the particle surface from effectively accommodating gaseous DMA molecules. Judging from the estimated DMA uptake coefficients, the retardation gradually intensified as the weight percentage of coating increased before leveling off, likely when the particle surface was completely covered by fresh or aged bulk OA. We propose that the accommodation of DMA on the particle coating is the rate-limiting step of DMA uptake. Intensive aging of the OA coating had little effect on the equilibrium particle-phase compositions but retarded DMA uptake.

© 2017 American Association for Aerosol Research     

Thermodynamic and kinetic behavior of glycerol aerosol

Glycerol and propylene glycol mixtures are common carrier solutions in electronic cigarettes. Aerosols produced from these mixtures will evaporate quickly in a dry environment due to their high volatility. In a humid environment, such as the lungs, the kinetics of evaporation and hygroscopic growth determine the evolution of aerosol plume glycerol. Here, we apply a temperature and relative humidity-controlled hygroscopicity/volatility tandem differential mobility analyzer system to study the growth and evaporation kinetics of glycerol aerosol over a wide range of temperature, relative humidity, and residence times. Results show that at dry conditions glycerol aerosols evaporate within seconds at temperatures warmer than 20°C and that the accommodation coefficient of glycerol vapor on dry glycerol particles is 0.8. Under humidified conditions, the mutual depression of vapor pressures of the aqueous glycerol/water solution slows the glycerol evaporation rate consistent with thermodynamic and kinetic model predictions. Model calculations show that water vapor aided condensation of glycerol can occur at high relative humidity for glycerol vapor concentrations that result in glycerol particle evaporation under dry conditions. The combined results will help with constraining computational modules that model the evolution of glycerol-containing aerosols along a prescribed thermodynamic trajectory.

Copyright © 2016 American Association for Aerosol Research     

Investigation of the size of the incandescent incipient soot particles in premixed sooting and nucleation flames of n-butane using LII,HIM, and 1 nm-SMPS

Laser-induced incandescence (LII) measurements were conducted to explore the ability of LII to detect small soot particles of less than 10 nm in two sooting flat premixed flames of n-butane: a so-called nucleation flame obtained at a threshold equivalence ratio Φ = 1.75, in which the incipient soot particles undergo only minor soot surface growth along the flame, and a more sooting flame at Φ = 1.95. Size measurements were obtained by modeling the time-resolved LII signals detected using 1064 nm laser excitation. Spectrally-resolved LII signals collected in the nucleation flame display a similar blackbody-like behavior as mature soot. Soot particle temperature was determined from spectrally-resolved detection. LII modeling was conducted using parameters either relevant to those of mature soot or derived from fitting the modeled results to the experimental LII data. Particle size measurements were also carried out using (1) ex situ analysis by helium-ion microscopy (HIM) of particles sampled thermophoretically and (2) online size distribution analysis of microprobe-sampled particles using a 1 nm-SMPS. The size distributions of the incipient soot particles, found in the nucleation flame and in the early soot region of the Φ = 1.95 flame, derived from time-resolved LII signals are in good agreement with HIM and 1 nm-SMPS measurements and are in the range of 2–4 nm. The thermal and optical properties of incipient soot were found to be not radically different from those of mature soot commonly used in LII modeling. This explains the ability of incipient soot particles to produce continuous thermal emissions in the visible spectrum. This study demonstrates that LII is a promising in situ optical particle sizing technique that is capable of detecting incipient soot as small as about 2.5 nm and potentially 2 nm and resolving small changes in soot sizes below 10 nm.

© 2017 American Association for Aerosol Research     

Humidity,density, and inlet aspiration efficiency correction improve accuracy of a low-cost sensor during field calibration at a suburban site in the North-Western Indo-Gangetic plain (NW-IGP)

Abstract

Low-cost particulate matter (PM) sensors are now widely used by concerned citizens to monitor PM exposure despite poor validation under field conditions. Here, we report the field calibration of a modified version of the Laser Egg (LE), against Class III US EPA Federal Equivalent Method PM₁₀ and PM_2.5 β-attenuation analyzers. The calibration was performed at a site in the north-western Indo-Gangetic Plain from 27 April 2016 to 25 July 2016. At ambient PM mass loadings ranging from <1–838?µg m^?3 and <1–228?µg m^?3 for PM₁₀ and PM_2.5, respectively, measurements of PM₁₀, PM_2.5 from the LE were precise, with a Pearson correlation coefficient (r) >0.9 and a percentage coefficient of variance (CV) <12%. The original Mean Bias Error (MBE) of ～?90?µg m^?3 decreased to ?30.9?µg m^?3 (Sensor 1) and ?23.2?µg m^?3 (Sensor 2) during the summer period (27 April–15 June 2016) after correcting for particle density and aspiration losses. During the monsoon period (16 June–25 July 2016) the MBE of the PM_2.5 measurements decreased from 19.1?µg m^?3 to 8.7?µg m^?3 and from 28.3?µg m^?3 to 16.5?µg m^?3 for Sensor 1 and Sensor 2, respectively, after correcting for particle density and hygroscopic growth. The corrections reduced the overall MBE to <20?µg m^?3 for PM₁₀ and <3?µg m^?3 for PM_2.5, indicating that modified version of the LE could be used for ambient PM monitoring with appropriate correction and meteorological observations. However, users of the original product may underestimate their PM₁₀ exposure.

Copyright © 2020 American Association for Aerosol Research     

Atmospheric particle composition-hygroscopic growth measurements using an in-series hybrid tandem differential mobility analyzer and aerosol mass spectrometer

The ability of atmospheric particles to absorb water has extensive climate, atmospheric chemistry, and health implications, and considerable effort has gone into determining relationships between particle composition and hygroscopicity. Parallel techniques, in which co-located composition and hygroscopicity measurements are combined to infer composition-hygroscopicity relationships, may not detect the influence of external mixtures. Previous in-line measurements have been limited to single-particle composition or a limited analyte range, and are often non-quantitative and/or offline. Here, we present for the first time in-series, online, quantitative hygroscopicity-composition measurements using a Brechtel Manufacturing, Inc. Hybrid Tandem Differential Mobility Analyzer and an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This technique is first verified using laboratory-generated external particle mixtures, then extended to ambient measurements at a seaside sampling side at the Hong Kong University of Science and Technology. The technique successfully separated laboratory-generated particles of differing hygroscopicities and showed promise for atmospheric particles, though high mass attenuation endemic to the HTDMA dual size selection limits application to environments with at least ～14–41 μg/m³ of particulate mass, depending on composition.

Copyright © 2017 American Association for Aerosol Research     

Laboratory study of the generation of nanoparticles from tire tread

An experimental study was carried out to investigate the formation process of airborne nanoparticles from tire tread. The formation of nanoparticles by volatilization of the tire tread was simulated in a reaction chamber. The number concentration of nanoparticles in the reaction chamber suddenly increased when the tire tread surface temperature reached above 160°C. The generated nanoparticles have a unimodal distribution and the number of nanoparticles increased as the heating rate increased. The geometric mean diameter and size distribution of the generated particles can be controlled by adjusting the cooling rate since the cooling rate is directly related to the growth of particles. From the morphological and elemental analyses, the main components of the tire nanoparticles were C, O, S, and Si and the particles had an irregular shape. Based on these observations, we concluded that the formation mechanism of nanoparticles from the tire tread was volatilization and condensation of the organic materials in the tire tread.

Copyright © 2017 American Association for Aerosol Research     

Control of the radial distribution of chemical components in spray-dried crystalline microparticles

The process of particle formation from evaporating droplets containing more than one solute was studied. Two-component microparticles were produced using a piezoceramic dispenser with an inner diameter of 30 µm. Initial droplets had a diameter in the range of 70–85 µm and contained sodium nitrate and potassium nitrate in different molar ratios of 30:70, 50:50, and 70:30, corresponding to weight ratios of 26.5:73.5, 45.7:54.3, and 66.2:33.8, in the form of aqueous solutions with initial concentrations of 1 or 10 mg/ml. The monodisperse droplets were dried in a dry laminar gas flow with temperatures of 50°C or 100°C. Different initial conditions affected the particle formation process and the particle morphology. The diameter of the final dried microparticles ranged from 4 to 10 µm. Their density varied from 1250 to 1950 mg/ml. The formulation and process conditions determined the distribution of chemical components in the dried microparticles, especially their surface composition as determined by energy-dispersive X-ray spectroscopy. The distribution of the chemical components was theoretically explained using characteristic times for the crystallization kinetics of the drying process. It was shown that the solute that reached supersaturation first formed most of the outer shell of the microparticles.

© 2016 American Association for Aerosol Research     

Highly sensitive nano-aerosol detection based on the whispering-gallery-mode in cylindrical optical fiber resonators

Highly sensitive detection of nanoscale aerosols, or nano-aerosols, is a difficult challenge. Here, we report a fiber optical technique that is capable of detecting trace-level nano-aerosols. Our method is based on monitoring the nano-aerosol-induced resonance shift due to the optical Whispering-Gallery-Mode (WGM) in a cylindrical optical fiber resonator. A nearly linear relationship between the WGM resonance shift and the aerosol coverage ratio of silica nanoparticles (40–50 nm dia.) on the fiber resonator was identified in the low coverage regime. Our experimental results imply sensitivity at the level of ～2 nanoparticles per μm² deposited on the fiber resonator, which corresponds to pg-level sensitivity in the total aerosol mass within the effective detection area. The response of this fiber optical sensor is further confirmed by using silica nanoparticles deposited on the fiber surface via electrostatic self-assembly. The fiber optical technique for nanoparticle detection may ultimately lead to an instrument capable of real-time in situ aerosol detection with ultrahigh sensitivity.

Copyright © 2016 American Association for Aerosol Research     

Aerosolization of colloidal nanoparticles by a residual-free atomizer

Abstract

A new residual-free atomizer was designed to transfer colloidal nanoparticles measuring less than 100?nm into aerosol phase. Miniaturization of droplet size distribution successfully reduced background aerosol concentration of particles sized greater than 2.5?nm to 400 particles·mL^?1 of gas, which corresponded to an NaCl-equivalent impurity concentration of less than 100?ppb. Direct injection of colloid suspension enabled precise control of aerosol number concentrations by colloidal concentration (10⁵–10¹¹ particles·mL^?1 of liquid). Correlations between the size distributions of colloid and aerosol were also investigated using aqueous suspensions of the standard nanoparticles sized 10–100?nm. It was found that the aerosol size distribution was in very good agreement (i.e., less than 1?nm accuracy) with that measured by scanning electron microscopy.

Copyright © 2020 American Association for Aerosol Research     

Instant acquisition of high resolution mobility spectra in a differential mobility analyzer with 100 independent ion collectors: Instrument calibration

Abstract

A parallel plate differential mobility analyzer (DMA) having 100 independent current collectors is calibrated to relate the axial distances L_n between the inlet slit and the detector position to the particle mobility Z at given voltage difference V and sheath gas flow rate Q. Calibrating species are tetraheptylammonium bromide clusters (THABr) and polyethylene glycol (PEG35k, 5?nm in diameter), generated by a bipolar electrospray source, and purified in a cylindrical DMA. Gaussian fitting of the raw discrete mobility spectra in the form of ion current I_n versus collector position L_n , I_n (L_n ), yield the mean value L_o of the collector position maximizing the signal for a given ion. The many (Z,V,L_o ) triads obtained at given Q from many different DMA voltages and standard mobilities collapse into a single 1/(Z_iV_j ) vs L_o curve when slight adjustments are made to the Z_i . For different flow rates, Q/(Z_iV_j ) vs. L_o curves collapse also, as long as the peaks are moderately narrow. However, for sufficiently small Q/Z, the THABr cluster peaks become broad, and the curves Q/(Z_iV_j ) vs. L_o cease to collapse precisely. In contrast, the data for PEG show that this behavior is not a low-Q (Reynolds number) effect from the growth of the two lateral boundary layers, but is rather due to the broad and non-Gaussian peak shapes obtained at low Q or high Z. The calibration is accordingly unaffected by the Reynolds number. This simplicity was unexpected, given the three-dimensional flow in this DMA with growing lateral boundary layers.

Copyright © 2020 American Association for Aerosol Research     

Experimental study of oil particle emission rate and size distribution during milling

Metalworking fluids (MWFs) used in milling generate oil particles through impaction, action of centrifugal forces and evaporation/condensation mechanisms. The oil particles suspended in the factory atmosphere can affect the health of the labor force. In order to study the emission properties of these oil particles, this work investigates the oil particle emission rate and size distribution during milling using an environmental chamber method. Two commonly used operating modes for MWFs were selected, the minimum quantity lubrication (MQL) mode (40?ml/h) and the cooling mode (1 m³/h). The cooling mode without cutting was studied separately for comparison with the cooling mode with cutting. The results show that the oil particle emission rate in milling ranges from 7.2 to 641?mg/h, and the size distribution ranges from 0.265 to 12.5?µm. Evaporation/condensation is the main mechanism in the MQL mode. The majority of oil particles formed by evaporation/condensation are in the range of 0.265 to 1.8?µm. As the tool rotation speed increases, the particle emission rate increases, while the mass mean diameter (MMD) and the sauter mean diameter (SMD) decrease. Oil particles are mainly generated by the action of centrifugal force in the cooling mode, and mainly distributed in the range of 1.8 to 12.5?µm. The particle emission rate increases with the tool rotation speed, and the particle MMD and SMD increase with the tool rotation speed only in the cooling mode without cutting. The particle emission rate ranging from 1.8 to 12.5?µm, as well as PM5 and PM10, are a polynomial function of the square of tool rotation speed during the cooling mode. The coefficient of determination (R²) is above 0.99.

© 2018 American Association for Aerosol Research