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Estimation of carcinogenic potency based on analysis of 16 polycyclic aromatic hydrocarbons (PAHs) ranked by U.S. Environmental Protection Agency (EPA) is the most popular approach within scientific and environmental air quality management communities. The majority of PAH monitoring projects have been focused on particle-bound PAHs, ignoring the contribution of gas-phase PAHs to the toxicity of PAH mixtures in air samples. In this study, we analyzed the results of 13 projects in which 88 PAHs in both gas and particle phases were collected from different sources (biomass burning, mining operation, and vehicle emissions), as well as in urban air. The aim was to investigate whether 16 particle-bound U.S. EPA priority PAHs adequately represented health risks of inhalation exposure to atmospheric PAH mixtures. PAH concentrations were converted to benzo(a)pyrene-equivalent (BaPeq) toxicity using the toxic equivalency factor (TEF) approach. TEFs of PAH compounds for which such data is not available were estimated using TEFs of close isomers. Total BaPeq toxicities (∑88BaPeq) of gas- and particle-phase PAHs were compared with BaPeq toxicities calculated for the 16 particle-phase EPA PAH (∑16EPABaPeq). The results showed that 16 EPA particle-bound PAHs underrepresented the carcinogenic potency on average by 85.6% relative to the total (gas and particle) BaPeq toxicity of 88 PAHs. Gas-phase PAHs, like methylnaphthalenes, may contribute up to 30% of ∑88BaPeq. Accounting for other individual non-EPA PAHs (i.e., benzo(e)pyrene) and gas-phase PAHs (i.e., naphthalene, 1- and 2-methylnaphthalene) will make the risk assessment of PAH-containing air samples significantly more accurate.

Light-absorbing organic carbon aerosol – colloquially known as brown carbon (BrC) – is emitted from combustion processes and has a brownish or yellowish visual appearance, caused by enhanced light absorption at shorter visible and ultraviolet wavelengths (0.3 µm≲λ≲0.5 µm). Recently, optical properties of atmospheric BrC aerosols have become the topic of intense research, but little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo, which can alter the resulting radiative forcing and in-snow photochemistry. Wildland fires in close proximity to the cryosphere, such as peatland fires that emit large quantities of BrC, are becoming more common at high latitudes, potentially affecting nearby snow and ice surfaces. In this study, we describe the artificial deposition of BrC aerosol with known optical, chemical, and physical properties onto the snow surface, and we monitor its spectral radiative impact and compare it directly to modeled values. First, using small-scale combustion of Alaskan peat, BrC aerosols were artificially deposited onto the snow surface. UV–Vis absorbance and total organic carbon (TOC) concentration of snow samples were measured for samples with and without artificial BrC deposition. These measurements were used to first derive a BrC (mass) specific absorption (m2 g−1) across the UV–Vis spectral range. We then estimate the imaginary part of the refractive index of deposited BrC aerosol using a volume mixing rule. Single-particle optical properties were calculated using Mie theory, and these values were used to show that the measured spectral snow albedo of snow with deposited BrC was in general agreement with modeled spectral snow albedo using calculated BrC optical properties. The instantaneous radiative forcing per unit mass of total organic carbon deposited to the ambient snowpack was found to be 1.23 (+0.14/-0.11) W m−2 per part per million (ppm). We estimate the same deposition onto a pure snowpack without light-absorbing impurities would have resulted in an instantaneous radiative forcing per unit mass of 2.68 (+0.27/-0.22) W m−2 per ppm of BrC deposited.

Starch is a polysaccharide that is abundantly found in nature and is generally used as an energy source and energy storage in many biological and environmental processes. Naturally, starch tends to be in miniscule amounts, creating a necessity for quantitative analysis of starch in low-concentration samples. Existing studies that are based on the spectrophotometric detection of starch using the colorful amylose–iodine complex lack a detailed description of the analytical procedure and important parameters. In the present study, this spectrophotometry method was optimized, tested, and applied to studying starch content of atmospheric bioaerosols such as pollen, fungi, bacteria, and algae, whose chemical composition is not well known. Different experimental parameters, including pH, iodine solution concentrations, and starch solution stability, were tested, and method detection limit (MDL) and limit of quantification (LOQ) were determined at 590 nm. It was found that the highest spectrophotometry signal for the same starch concentration occurs at pH 6.0, with an iodine reagent concentration of 0.2%. The MDL was determined to be 0.22 μg/mL, with an LOQ of 0.79 μg/mL. This optimized method was successfully tested on bioaerosols and can be used to determine starch content in low-concentration samples. Starch content in bioaerosols ranged from 0.45 ± 0.05 (in bacteria) to 4.3 ± 0.06 μg/mg (in fungi).

Semivolatile organic compounds (SVOCs) emitted from open biomass burning (BB) can contribute to chemical and physical properties of atmospheric aerosols and also may cause adverse health effects. The polar fraction of SVOCs is a prominent part of BB organic aerosols, and thus it is important to characterize the chemical composition and reactivity of this fraction. In this study, globally and regionally important representative fuels (Alaskan peat, Moscow peat, Pskov peat, eucalyptus, Malaysian peat, and Malaysian agricultural peat) were burned under controlled conditions using the combustion chamber facility at the Desert Research Institute (DRI). Gas- and particle-phase biomass-burning emissions were aged in an oxidation flow reactor (OFR) to mimic 5–7 d of atmospheric aging. Fresh and OFR-aged biomass-burning aerosols were collected on Teflon-impregnated glass fiber filters (TIGF) in tandem with XAD resin media for organic carbon speciation. The polar fraction extracted with dichloromethane and acetone was analyzed with gas chromatography mass spectrometry (GC-MS) for 84 polar organic compounds – including mono- and dicarboxylic acids, methoxylated phenols, aromatic acids, anhydrosugars, resin acids, and sterols. For all these compounds, fuel-based emission factors (EFs) were calculated for fresh and OFR-aged samples. The carbon mass of the quantified polar compounds was found to constitute 5 % to 7 % of the total organic compound mass. A high abundance of methoxyphenols (239 mg kg−1 for Pskov peat; 22.6 % of total GC-MS characterized mass) and resin acids (118 mg kg−1 for Alaskan peat; 14.5 % of total GC-MS characterized mass) was found in peat-burning emissions (smoldering combustion). The concentration of some organic compounds (e.g., tetracosanoic acid) with a molecular weight (MW) above 350 g mol−1 decreased after OFR aging, while abundances of low-MW compounds (e.g., hexanoic acid) increased. This indicated a significant extent of fragmentation reactions in the OFR. Methoxyphenols decreased after OFR aging, while a significant increase (3.7 to 8.6 times) in the abundance of dicarboxylic acids emission factors (EFs), especially maleic acid (10 to 60 times), was observed. EFs for fresh and ratios from fresh-to-aged BB samples reported in this study can be used to perform source apportionment and predict processes occurring during atmospheric transport.

We present spatial measurements of particle volatility and mixing state at a site near a North Carolina interstate highway (I-40) applying several heating (thermodenuder; TD) experimental approaches. Measurements were conducted in summer 2015 and winter 2016 in a roadside trailer (10 m from road edge) and during downwind transects at different distances from the highway under favorable wind conditions using a mobile platform. Results show that the relative abundance of semi-volatile species (SVOCs) in ultrafine particles decreases with downwind distance, which is consistent with the dilution and mixing of traffic-sourced particles with background air and evaporation of semi-volatile species during downwind transport. An evaporation kinetics model was used to derive particle volatility distributions by fitting TD data. While the TD-derived distribution apportions about 20–30 % of particle mass as semi-volatile (SVOCs; effective saturation concentration, C∗ ≥ 1µm−3) at 10 m from the road edge, approximately 10 % of particle mass is attributed to SVOCs at 220 m, showing that the particle-phase semi-volatile fraction decreases with downwind distance. The relative abundance of semi-volatile material in the particle phase increased during winter. Downwind spatial gradients of the less volatile particle fraction (that remaining after heating at 180 °C) were strongly correlated with black carbon (BC). BC size distribution and mixing state measured using a single-particle soot photometer (SP2) at the roadside trailer showed that a large fraction (70–80 %) of BC particles were externally mixed. Heating experiments with a volatility tandem differential mobility analyzer (V-TDMA) also showed that the nonvolatile fraction in roadside aerosols is mostly externally mixed. V-TDMA measurements at different distances downwind from the highway indicate that the mixing state of roadside aerosols does not change significantly (e.g., BC mostly remains externally mixed) within a few hundred meters from the highway. Our analysis indicates that a superposition of volatility distributions measured in laboratory vehicle tests and of background aerosol can be used to represent the observed partitioning of near-road particles. The results from this study show that exposures and impacts of BC and semi-volatile organics-containing particles in a roadside microenvironment may differ across seasons and under changing ambient conditions.

Use of electronic nicotine delivery systems (ENDS), such as electronic cigarettes (e-cigs), is increasing across the US population and is particularly troubling due to their adoption by adolescents, teens, and young adults. The industry's marketing approach for these instruments of addiction has been to promote them as a safer alternative to tobacco, a behavioral choice supporting smoking cessation, and as the 'cool' appearance of vaping with flavored products (e.g. tutti frutti, bubble gum, and buttered popcorn etc.). Thus, there is a clear need to better document the health outcomes of e-cig use in the oral cavity of the addicted chronic user. There appears to be an array of environmental toxins in the vapors, including reactive aldehydes and carbonyls resulting from the heating elements action on fluid components, as well as from the composition of chemical flavoring agents. The chemistry of these systems shows that the released vapors from the e-cigs frequently contain levels of environmental toxins that considerably exceed federal occupational exposure limits. Additionally, the toxicants in the vapors appear to be retained in the host fluids/tissues at levels often approximating 90% of the levels in the e-cig vapors. These water-soluble reactive toxins can challenge the oral cavity constituents, potentially contributing to alterations in the autochthonous microbiome and host cells critical for maintaining oral homeostasis. This review updates the existing chemistry/environmental aspects of e-cigs, as well as providing an overview of the somewhat limited data on potential oral health effects that could occur across the lifetime of daily e-cig users.

Several studies have shown the presence of aldehydes (i.e., formaldehyde, acrolein) in mainstream emissions of some e-cigarettes. For this reason, concerns have been raised regarding potential toxicity. The purpose of this research was to measure levels of carbonyls in exhaled breath of e-cigarette users during “vaping” sessions and estimate the respiratory tract (RT) uptake of specific aldehydes, including formaldehyde and acetaldehyde. We measured concentrations of 12 carbonyls in e-cigarette aerosols produced directly by e-cigarettes and in the exhaled breath of 12 participants (19 sessions). Carbonyls were sampled on 2,4-dinitrophenylhydrazine (DNPH) cartridges and analyzed with high performance liquid chromatography (HPLC) coupled with a UV/Vis photodiode detector. We found that in most cases, levels of aldehydes and methyl ethyl ketone (MEK) were significantly higher (2–125 times) in exhaled e-cigarette breaths than in pre-exposed breath. Exposure levels for the most abundant individual carbonyls in e-cigarette emissions—formaldehyde, acetaldehyde, acrolein—were between the limit of quantification (LOQ) and 24.4 μg·puff−1. The mean retention of formaldehyde in the respiratory tract was 99.7 ± 0.9% for all participants, while acetaldehyde retention was 91.6 ± 9.9%. Within the limitation of a small number of participants, our results showed that there is an increase in breath carbonyls during e-cigarette use.

The below-cloud irradiance in The Netherlands increased by over 10 Wm−2 in the past half century. It was hypothesized that this could be due to a decrease in the aerosol serving as cloud condensation nuclei, on which the cloud droplets form, in the following way. With unchanged macrophysics, clouds with a lower number of droplets are less reflective, in other words, they transmit more solar radiation. This hypothesis cannot be substantiated with data because of a generic absence of long-term information on cloud droplet number concentrations (CDNCs) worldwide. To assess the historic trend in CDNC, we used the Boucher and Lohmann (B&L) empirical relationship between CDNC and the mass concentration of the water-attracting hygroscopic aerosol components. The B&L parameterization was tested and validated with observations from the CHIEF cloud chamber, in which the formation of marine stratocumulus, the most frequent cloud type in The Netherlands, is simulated. This study will focus on summer periods because the irradiance governs the yearly average at this latitude. The summer trend of sulfate, the most dominant hygroscopic component of observed aerosol mass concentration, was analyzed with EBAS data from 1972 onwards. The average summer CDNCs were then calculated via the B&L parameterization, showing an upper limit of 380 cm−3 in the 1970s and decreasing to around 200 cm−3 in the 2010s. The associated increase in transmission for thin marine stratocumulus without overlying clouds would be, at most, 3.5 W m−2. Unobstructed stratocumuli occur only part of the time, and the change in irradiance based on the reduction in cloud droplet number is certainly small in comparison to the empirically derived trend of 10 W m−2.

This study aims to understand the effects of wildfires in sagebrush ecosystem on soil properties by examining connections between Soil Water Repellency (SWR), reflectance, and chemistry. Ash and burned soil samples were collected after performing laboratory burns of three common sagebrush plants: sagebrush, rabbitbrush, and bitterbrush. The collected samples were analyzed for their physical properties, including SWR measured by Water Drop Penetration Time (WDPT) and Apparent Contact Angle (ACA), and solar spectral reflectance in the wavelength range of 350 to 2500 nm. Chemical functional groups of the samples were analyzed using Fourier-Transform Infrared (FTIR) spectroscopy. WDPT and ACA values were in the range of 1 to 600 s and ~10° to 88°, respectively, for all three tested fuels. The FTIR analysis showed a decrease (~2 to 4 times) in the ratio of COO−/C=C signals for the burned soil samples compared to the unburned soil samples. Overall, increase in temperature and ACA levels for the samples of burned and burned soil from a 2 cm depth led to increased formation of non-polar compounds with C=C functional groups, and decarboxylation.

While western U.S. wildfires have increased in intensity and scale, their impacts on soil chemical composition and hydraulic processes have received little attention, despite increasing erosion, surface runoff and flooding. The relationships between biomass-burning emissions, composition of the soil, fire heat, and soil water repellency are fragmental and sometimes contradictory. Here, we characterized the water repellency of sand (soil surrogate) exposed to Jeffrey pine duff smoke under controlled laboratory conditions. Water drop penetration time (WDPT), effective contact angle, and relative sorptivity of exposed silica sand (soil surrogate) were determined. Sand samples treated with smoke and heat or with cold smoke showed severe-to-extreme water repellency (WDPT > 1020 s). Sand samples exposed to fulvic acid (surrogate for soil organic matter) showed strong water repellency (WDPT = 81 s) that increased to become severe (WDPT = 2305 s) after subsequent heating to 200 °C for two hours. All sand samples exposed to either fire emissions or fulvic acid showed WDPTs >81 s, effective contact angles between 78° and 87°, and relative sorptivities between 0.31 and 0.49 compared with the untreated sand samples, with a WDPT <0.5 s, effective contact angle of 48°, and relative sorptivity of 1. This indicates that the sorptivity-controlled water infiltration into treated sand is less than half of that into untreated sand.