Abstract. Ammonium-containing aerosols are a major component of wintertime air pollution in many densely populated regions around the world. Especially in mountain basins, the formation of persistent cold-air pools (PCAPs) can enhance particulate matter with diameters less than 2.5 µm (PM2.5) to levels above air quality standards. Under these conditions, PM2.5 in the Great Salt Lake region of northern Utah has been shown to be primarily composed of ammonium nitrate; however, its formation processes and sources of its precursors are not fully understood. Hence, it is key to understanding the emission sources of its gas phase precursor, ammonia (NH3). To investigate the formation of ammonium nitrate, a suite of trace gases and aerosol composition were sampled from the NOAA Twin Otter aircraft during the Utah Winter Fine Particulate Study (UWFPS) in January and February 2017. NH3 was measured using a quantum cascade tunable infrared laser differential absorption spectrometer (QC-TILDAS), while aerosol composition, including particulate ammonium (pNH4), was measured with an aerosol mass spectrometer (AMS). The origin of the sampled air masses was investigated using the Stochastic Time-Inverted Lagrangian Transport (STILT) model and combined with an NH3 emission inventory to obtain model-predicted NHx (=NH3+pNH4) enhancements. Enhancements represent the increase in NH3 mixing ratios within the last 24 h due to emissions within the model footprint. Comparison of these NHx enhancements with measured NHx from the Twin Otter shows that modelled values are a factor of 1.6 to 4.4 lower for the three major valleys in the region. Among these, the underestimation is largest for Cache Valley, an area with intensive agricultural activities. We find that one explanation for the underestimation of wintertime emissions may be the seasonality factors applied to NH3 emissions from livestock. An investigation of inter-valley exchange revealed that transport of NH3 between major valleys was limited and PM2.5 in Salt Lake Valley (the most densely populated area in Utah) was not significantly impacted by NH3 from the agricultural areas in Cache Valley. We found that in Salt Lake Valley around two thirds of NHx originated within the valley, while about 30 % originated from mobile sources and 60 % from area source emissions in the region. For Cache Valley, a large fraction of NOx potentially leading to PM2.5 formation may not be locally emitted but mixed in from other counties.
Levels of volatile organic compounds (VOCs) in the indoor environment can be decreased by the use of "air cleaners", devices that remove VOCs by sorption and/or oxidative degradation. However, efficacies of these technologies for removing VOCs tend to be poorly constrained, as does the formation of oxidation byproducts. Here, we examine the influence of several oxidation-based air cleaners, specifically ones marketed as consumer-grade products, on the amounts and composition of VOCs. Experiments were conducted in an environmental chamber, with a suite of real-time analytical instruments to measure direct emissions, VOC removal efficacies (by the addition of either limonene and toluene), and byproduct formation. We find that the air cleaners themselves can be a source of organic gases, that removal efficacy can be exceedingly variable, and that VOC loss is primarily driven by physical removal in some cleaners. When oxidative degradation of VOCs was observed, it was accompanied by the formation of a range of oxidation byproducts, including formaldehyde and other oxygenates. These results indicate that some consumer-grade portable air cleaners can be ineffective in removing VOCs and that the air delivered may contain a range of organic compounds, due to direct emission and/or byproduct formation.
<p><strong>Abstract.</strong> Ammonium-containing aerosols are a major component of winter time air pollution in many densely populated regions around the world. Especially in mountain basins, the formation of persistent cold air pool (PCAP) periods can enhance particulate matter with diameters less than 2.5&#8201;&#956;m (PM<sub>2.5</sub>) to levels above air quality standards. Under these conditions, PM<sub>2.5</sub> in the Great Salt Lake Region of northern Utah has been shown to be primarily composed of ammonium nitrate, however, its formation processes and sources of its precursors are not fully understood. Hence, it is key to understand the emission sources of its gas-phase precursor, ammonia (NH<sub>3</sub>). To investigate the formation of ammonium nitrate, a suite of trace gases and aerosol composition were sampled from the NOAA Twin Otter aircraft during the Utah Winter Fine Particulate Study (UWFPS) in January and February 2017. NH<sub>3</sub> was measured using a Quantum Cascade Tunable Infrared Laser Differential Absorption Spectrometer (QC-TILDAS), while aerosol composition, including particulate ammonium (pNH<sub>4</sub>), was measured with an aerosol mass spectrometer (AMS). The origin of the sampled air masses was investigated using the Stochastic Time-Inverted Lagrangian Transport (STILT) model and combined with an NH<sub>3</sub> emission inventory to obtain model-predicted NH<sub>x</sub> (=&#8201;NH<sub>3</sub>&#8201;+&#8201;pNH<sub>4</sub>) enhancements. Comparison of these NH<sub>x</sub> enhancements with measured NH<sub>x</sub> from the Twin Otter shows that modelled values are a factor of 1.6 to 4.4 lower for the three major valleys in the region. Among these, the underestimation is largest for Cache Valley, an area with intensive agricultural activities. We find that one explanation for the underestimation of wintertime emissions may be the seasonality factors applied to NH<sub>3</sub> emissions from livestock. An investigation of inter-valley exchange revealed that transport of NH<sub>3</sub> between major valleys was limited and PM<sub>2.5</sub> in Salt Lake Valley (the most densely populated area in Utah) was not significantly impacted by NH<sub>3</sub> from the agricultural areas in Cache Valley. We found that in Salt Lake Valley around two thirds of NH<sub>x</sub> originated within the valley, while about 30&#8201;% originated from mobile source and 60&#8201;% from area source emissions in the region. For Cache Valley, a large fraction of NO<sub>x</sub> potentially leading to PM<sub>2.5</sub> formation may not be locally emitted but mixed in from other counties.</p>
Background. Polycyclic aromatic hydrocarbons (PAHs) emitted from combustion sources are known to be mutagenic, with more potent species also being carcinogenic. Previous studies show that PAHs can undergo complex transformations both in the body and in the atmosphere, yet these transformation processes are generally investigated separately. Objectives. Drawing from the literature in atmospheric chemistry and toxicology, we highlight the parallel transformations of PAHs that occur in the atmosphere and the body and discuss implications for public health. We also examine key uncertainties related to the toxicity of atmospheric oxidation products of PAHs and explore critical areas for future research. Discussion. We focus on a key mode of toxicity for PAHs, in which metabolic processes (driven by cytochrome P450 enzymes), leads to the formation of oxidized PAHs that can damage DNA. Such species can also be formed abiotically in the atmosphere from natural oxidation processes, potentially augmenting PAH toxicity by skipping the necessary metabolic steps that activate their mutagenicity. Despite the large body of literature related to these two general pathways, the extent to which atmospheric oxidation affects a PAH’s overall toxicity remains highly uncertain. Combining knowledge and promoting collaboration across both fields can help identify key oxidation pathways and the resulting products that impact public health. Conclusions. Cross-disciplinary research, in which toxicology studies evaluate atmospheric oxidation products and their mixtures, and atmospheric measurements examine the formation of compounds that are known to be most toxic. Close collaboration between research communities can help narrow down which PAHs, and which PAH degradation products, should be targeted when assessing public health risks. https://doi.org/10.1289/EHP9984
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