Spatiotemporal variability in the oxidative potential of ambient fine particulate matter in the Midwestern United States

<p>We assessed the oxidative potential (OP) of both water-soluble and methanol-soluble fractions of ambient fine particulate matter (PM<span class="inline-formula"><sub>2.5</sub></span>) in the Midwestern United States. A large set of PM<span class="in...

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Autores principales: H. Yu, J. V. Puthussery, Y. Wang, V. Verma
Formato: article
Lenguaje:EN
Publicado: Copernicus Publications 2021
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Acceso en línea:https://doaj.org/article/cd769ee8c09943b58507bc47d79ec0e6
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Sumario:<p>We assessed the oxidative potential (OP) of both water-soluble and methanol-soluble fractions of ambient fine particulate matter (PM<span class="inline-formula"><sub>2.5</sub></span>) in the Midwestern United States. A large set of PM<span class="inline-formula"><sub>2.5</sub></span> samples (<span class="inline-formula"><i>N</i>=241</span>) was collected from five sites set up in different environments, i.e., urban, rural, and roadside, in Illinois, Indiana, and Missouri during May 2018–May 2019. Five acellular OP endpoints, including the consumption rate of ascorbic acid and glutathione in a surrogate lung fluid (SLF) (OP<span class="inline-formula"><sup>AA</sup></span> and OP<span class="inline-formula"><sup>GSH</sup></span>, respectively), dithiothreitol (DTT) depletion rate (OP<span class="inline-formula"><sup>DTT</sup></span>), and <span class="inline-formula"><span class="Radical">⚫</span>OH</span> generation rate in SLF and DTT (OP<span class="inline-formula"><sup>OH−SLF</sup></span> and OP<span class="inline-formula"><sup>OH−DTT</sup></span>, respectively), were measured for all PM<span class="inline-formula"><sub>2.5</sub></span> samples. PM<span class="inline-formula"><sub>2.5</sub></span> mass concentrations in the Midwestern US as obtained from these samples were spatially homogeneously distributed, while most OP endpoints showed significant spatiotemporal heterogeneity. Seasonally, higher activities occurred in summer for most OP endpoints for both water- and methanol-soluble extracts. Spatially, the roadside site showed the highest activities for most OP endpoints in the water-soluble extracts, while only occasional peaks were observed at urban sites in the methanol-soluble OP. Most OP endpoints showed similar spatiotemporal trends between mass- and volume-normalized activities across different sites and seasons. Comparisons between two solvents (i.e., water and methanol) showed that methanol-soluble OP generally had higher activity levels than corresponding water-soluble OP. Site-to-site comparisons of OP showed stronger correlations for methanol-soluble OP compared to water-soluble OP, indicating a better extraction of water-insoluble redox-active compounds from various emission sources into methanol. We found a weak correlation and inconsistent slope values between PM<span class="inline-formula"><sub>2.5</sub></span> mass and most OP endpoints. Moreover, the poor to moderate intercorrelations among different OP endpoints indicate different mechanisms of OP represented by these endpoints and thus demonstrate the rationale for analyzing multiple acellular endpoints for a better and more comprehensive assessment of OP.</p>