Iron is a limiting nutrient in about half of the world's oceans, and its most significant source is atmospheric deposition. To understand the pathways of iron solubilization during atmospheric transport, we exposed size segregated simulated marine aerosols to 5 ppm sulfur dioxide at arid (23 ± 1% relative humidity, RH) and marine (98 ± 1% RH) conditions. Relative iron solubility increased as the particle size decreased for goethite and hematite, while for magnetite, the relative solubility was similar for all of the fine size fractions (2.5-0.25 μm) investigated but higher than the coarse size fraction (10-2.5 μm). Goethite and hematite showed increased solubility at arid RH, but no difference (p > 0.05) was observed between the two humidity levels for magnetite. There was no correlation between iron solubility and exposure to SO2 in any mineral for any size fraction. X-ray absorption near edge structure (XANES) measurements showed no change in iron speciation [Fe(II) and Fe(III)] in any minerals following SO2 exposure. SEM-EDS measurements of SO2-exposed goethite revealed small amounts of sulfur uptake on the samples; however, the incorporated sulfur did not affect iron solubility. Our results show that although sulfur is incorporated into particles via gas-phase processes, changes in iron solubility also depend on other species in the aerosol.
Abstract. Iron is the most abundant transition element in airborne particulate matter (PM), primarily existing as Fe(II) or Fe(III). Generally, the fraction of water-soluble iron is greater in urban areas compared to areas dominated by crustal emissions. To better understand the origin of water-soluble iron in urban areas, tailpipe emission samples were collected from 32 vehicles with emission certifications of Tier 0 low emission vehicles (LEV I), Tier 2 low emission vehicles (LEV II), ultralow emission vehicles (ULEVs), super-ultralow emission vehicles (SULEVs), and partial-zero emission vehicles (PZEVs). The components quantified included gases, inorganic ions, elemental carbon (EC), organic carbon (OC), total metals, and water-soluble metals. Naphthalene and intermediate-volatility organic compounds (IVOCs) were quantified for a subset of vehicles. The IVOCs quantified contained 12 to 18 carbons and were divided into three subgroups: aliphatic, single-ring aromatic (SRA), and polar (material not classified as either aliphatic or SRA). Iron solubility in the tested vehicles ranged from 0 % to 82 % (average 30 %). X-ray absorption near-edge structure (XANES) spectroscopy showed that Fe(III) was the primary oxidation state in 14 of the 16 tested vehicles, confirming that the presence of Fe(II) was not the main driver of water-soluble Fe. The correlation of water-soluble iron with sulfate was insignificant, as was correlation with every chemical component except naphthalene and some C12–C18 IVOCs with R2 values as high as 0.56. A controlled benchtop study confirmed that naphthalene alone increases iron solubility from soils by a factor of 5.5 and that oxidized naphthalene species are created in the extract solution. These results suggest that the large driver in water-soluble iron from primary vehicle tailpipe emissions is related to the organic composition of the PM. We hypothesize that, during the extraction process, specific components of the organic fraction of the PM are oxidized and chelate the iron into water.
The ability of nanotechnology-enabled consumer sprays to inactivate bacteria has direct health implications. This research investigated the ability of six nanosilver-based consumer sprays to inactivate bacteria. We determined the minimal inhibitory concentrations (MICs) of the products by an agar dilution method, collected particles released from sprays onto bacterial films using impactors, and determined metal concentrations in the products using ICPMS. Also, the size of silver nanoparticles in the products' suspensions was determined using single particle (sp)ICPMS. Two of the six nanoproducts inhibited growth of and bacteria (MICs of 40,000 and 160,000 ppm). Collection of particles aerosolized from these two products onto films of the same bacteria inhibited bacterial growth; however, the mass concentration deposited onto bacterial films was lower than the MICs. Furthermore, these two nanoproducts had the lowest silver concentrations compared to the other four nanosilver products. Yet, they had the smallest nanosilver particles: mean size of ~20 to 30 nm vs. ~45 nm for the other products. Their suspensions were more acidic (pH ~3-5) and had higher concentrations of zinc and magnesium compared to other products. This research illustrates that some consumer nanoproducts have antibacterial potential and may affect our microbiota. Yet, the inactivation potential cannot solely be presumed based on the nanosilver presence and concentration in the product; the final nanoproduct's form, including its matrix, must be considered. As nanomaterials are increasingly incorporated into consumer goods, this research highlights the need to investigate final-form consumer nanoproducts and their potential to affect our microbial environment.
<p><strong>Abstract.</strong> Iron is the most abundant transition element in airborne PM, primarily existing as Fe(II) or Fe(III). Generally, the fraction of water-soluble iron is greater in urban areas compared to areas dominated by crustal emissions. To better understand the origin of water-soluble iron in urban areas, tail-pipe emission samples were collected from 32 vehicles with emission certifications of Tier 0, low emission vehicles (LEV I), tier two low emission vehicles (LEV II), ultralow emission vehicles (ULEV), superultra-low emission vehicles (SULEV), and partial-zero emission vehicles (PZEV). Components quantified included gases, inorganic ions, EC/OC, total metals and water-soluble metals. In addition, naphthalene and various classes of C12&#8211;C18 intermediate volatility organic compounds (IVOC) were quantified for a subset of vehicles: aliphatic, single ring aromatic (SRA), and polar (material not classified as either aliphatic or SRA). Iron solubility in the tested vehicles ranged from 0&#8211;82&#8201;% (average&#8201;=&#8201;30&#8201;%). X-ray absorption near edge structure (XANES) spectroscopy showed that Fe(III) was the primary oxidation state in 14 of the 16 tested vehicles, confirming that the presence of Fe(II) was not the main driver of water-soluble Fe. Correlation of water-soluble iron to sulfate was insignificant, as was correlation to every chemical component, except to naphthalene and some C12&#8211;C18 IVOCs with R<sup>2</sup> values as high as 0.56. A controlled benchtop study confirmed that naphthalene, alone, increases iron solubility from soils by a factor of 5.5 and that oxidized naphthalene species are created in the extract solution. These results suggest that the large driver in water-soluble iron from primary vehicle tail-pipe emissions is related to the organic composition of the PM, indicating the organic fraction of the PM influences the behavior and solubility of iron.</p>
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