Atmospheric combustion particles, such as fly ash emitted from coal-fired power plants, are a potential source of atmospheric iron, with significant implications in climate and global biogeochemical cycles. While the iron content and speciation of fly ash depend closely on the source region and combustion process, few studies have been carried out comparing the atmospheric processing of fly ash produced from coal-fired power plants in different regions. In this study, we present an investigation of iron dissolution in acidic aqueous solutions: HNO 3 and HCl at pH 1 and pH 2 under daytime and nighttime conditions for three fly ash samples from three different sources: United States (USFA), Central Europe (EUFA), and India fly ash (INFA). Iron mobility and speciation depend on the source region and the combustion efficiency that generates fly ash. In HCl suspensions, proton-promoted mechanisms lead to larger fractions of aqueous-phase iron leached from fly ash particles, with poorly combusted samples providing significant fractions of Fe 2+ . In HNO 3 suspensions, a surface-mediated redox reaction suppresses the mobility of Fe 2+ , leading to the formation of nitrites. In the presence of solar radiation, previously unrecognized pathways of atmospheric processing enhance the formation Fe 2+ and nitrous acid from combustion particles. The information provided herein could be significant to increase our understanding of the effects of combustion particles in the atmospheric chemical balance regarding iron and nitrites.
Aerosols significantly influence atmospheric processes such as cloud nucleation, heterogeneous chemistry, and heavy-metal transport in the troposphere. The chemical and physical complexity of atmospheric aerosols results in large uncertainties in their climate and health effects. In this article, we review recent advances in scientific understanding of aerosol processes achieved by the application of quantum chemical calculations. In particular, we emphasize recent work in two areas: new particle formation and heterogeneous processes. Details in quantum chemical methods are provided, elaborating on computational models for prenucleation, secondary organic aerosol formation, and aerosol interface phenomena. Modeling of relative humidity effects, aerosol surfaces, and chemical kinetics of reaction pathways is discussed. Because of their relevance, quantum chemical calculations and field and laboratory experiments are compared. In addition to describing the atmospheric relevance of the computational models, this article also presents future challenges in quantum chemical calculations applied to aerosols.
Atmospheric nitrous acid (HONO), a trace atmospheric gas, is often underestimated in global atmospheric models due to the poor understanding of its daytime sources and sinks. HONO is known to accumulate during nighttime and undergo rapid photodissociation during the day to form NO and highly reactive OH radical, making it important to have accurate atmospheric HONO estimations. Despite its rapid photolysis, recent field observations have found quasi-steady-state concentrations of HONO at midday, suggesting photolytic HONO formation pathways to replenish daytime atmospheric HONO. Recent studies suggest that the presence of complex organic photosensitizers in atmospheric aerosols converts atmospheric NO 2 into HONO. To better understand the effect of environmental photosensitizers in daytime mechanisms of HONO formation, we present here laboratory studies on the heterogeneous photolytic reduction of NO 2 by humic acid films, a proxy for organic chromophoric compounds. The effect of pH and Cl − in the photosensitized formation of HONO and other nitrogen-containing gases is also investigated. A dual Fourier transform infrared (FTIR) system is utilized to simultaneously perform in situ analysis of condensed-phase reactants and gas-phase products. We find that the rate of HONO formation is faster at lower pHs. Nitrogen incorporation in the complex organic chromophore is observed, suggesting a competing pathway that results in suppressed daytime formation of nitrogenous gases. Significantly, the presence of chloride ions also leads to the organic-mediated photolytic formation of nitrosyl chloride (ClNO), a known precursor of HONO. Overall, this work shows that organic acid photosensitizers can reduce adsorbed NO 2 to form HONO, ClNO, and NO while simultaneously incorporating nitrogen into the organic chromophores present in aerosol.
Adhesion is a crucial characteristic of epithelial cells to form barriers to pathogens and toxic substances from the environment. Epithelial cells attach to each other using intercellular junctions on the lateral membrane, including tight and adherent junctions, as well as the Na+,K+-ATPase. Our group has shown that non-adherent chinese hamster ovary (CHO) cells transfected with the canine β1 subunit become adhesive, and those homotypic interactions amongst β1 subunits of the Na+,K+-ATPase occur between neighboring epithelial cells. Ouabain, a cardiotonic steroid, binds to the α subunit of the Na+,K+-ATPase, inhibits the pump activity and induces the detachment of epithelial cells when used at concentrations above 300 nM. At nanomolar non-inhibiting concentrations, ouabain affects the adhesive properties of epithelial cells by inducing the expression of cell adhesion molecules through the activation of signaling pathways associated with the α subunit. In this study, we investigated whether the adhesion between β1 subunits was also affected by ouabain. We used CHO fibroblasts stably expressing the β1 subunit of the Na+,K+-ATPase (CHO β1), and studied the effect of ouabain on cell adhesion. Aggregation assays showed that ouabain increased the adhesion between CHO β1 cells. Immunofluorescence and biotinylation assays showed that ouabain (50 nM) increases the expression of the β1 subunit of the Na+,K+-ATPase at the cell membrane. We also examined the effect of ouabain on the activation of signaling pathways in CHO β1 cells, and their subsequent effect on cell adhesion. We found that cSrc is activated by ouabain and, therefore, that it likely regulates the adhesive properties of CHO β1 cells. Collectively, our findings suggest that the β1 subunit adhesion is modulated by the expression levels of the Na+,K+-ATPase at the plasma membrane, which is regulated by ouabain.
Small uncrewed aerial systems (sUASs) have the potential to serve as ideal platforms for high spatial and temporal resolution wildfire measurements to complement aircraft and satellite observations, but typically have very limited payload capacity. Recognizing the need for improved data from wildfire management and smoke forecasting communities and the potential advantages of sUAS platforms, the Nighttime Fire Observations eXperiment (NightFOX) project was funded by the US National Oceanic and Atmospheric Administration (NOAA) to develop a suite of miniaturized, relatively low-cost scientific instruments for wildfire-related measurements that would satisfy the size, weight and power constraints of a sUAS payload. Here we report on a remote sensing system developed under the NightFOX project that consists of three optical instruments with five individual sensors for wildfire mapping and fire radiative power measurement and a GPS-aided inertial navigation system module for aircraft position and attitude determination. The first instrument consists of two scanning telescopes with infrared (IR) channels using narrow wavelength bands near 1.6 and 4 µm to make fire radiative power measurements with a blackbody equivalent temperature range of 320–1500 °C. The second instrument is a broadband shortwave (0.95–1.7 µm) IR imager for high spatial resolution fire mapping. Both instruments are custom built. The third instrument is a commercial off-the-shelf visible/thermal IR dual camera. The entire system weighs about 1500 g and consumes approximately 15 W of power. The system has been successfully operated for fire observations using a Black Swift Technologies S2 small, fixed-wing UAS for flights over a prescribed grassland burn in Colorado and onboard an NOAA Twin Otter crewed aircraft over several western US wildfires during the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field mission.
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