Assessing the oxidative potential of PAHs in ambient PM2.5 using the DTT consumption assay
2021
Kramer, Amber L. | Dorn, Shelby | Perez, Allison | Roper, Courtney | Titaley, Ivan A. | Cayton, Kaylee | Cook, Ronald P. | Cheong, Paul H-Y | Massey Simonich, Staci L.
The oxidative potential (OP) of atmospheric fine particulate matter (PM₂.₅) has been linked to organic content, which includes polycyclic aromatic hydrocarbons (PAHs). The OP of 135 individual PAHs (including six subclasses) was measured using the dithiolthreitol (DTT) consumption assay. The DTT assay results were used to compute the concentration of each PAH needed to consume 50% of the DTT concentration in the assay (DTT₅₀), and the reduction potential of the PAHs (ΔGᵣₓₙ). Computed reduction potential results were found to match literature reduction potential values (r² = 0.97), while DTT₅₀ results had no correlations with the computed ΔGᵣₓₙ values (r² < 0.1). The GINI equality index was used to assess the electron distribution across the surface of unreacted and reacted PAHs. GINI values correlated with ΔGᵣₓₙ in UPAH, HPAH, and OHPAH subclasses, as well as with all 135 PAHs in this study but did not correlate with DTT₅₀, indicating that electron dispersion is linked to thermodynamic reactions and structural differences in PAHs, but not linked to the OP of PAHs. Three ambient PM₂.₅ filters extracts were measured in the DTT assay, alongside mixtures of analytical standards prepared to match PAH concentrations in the filter extracts to test if the OP follows an additive model of toxicity. The additive prediction model did not accurately predict the DTT consumption in the assay for any of the prepared standard mixtures or ambient PM₂.₅ filter extracts, indicating a much more complex model of toxicity for the OP of PAHs in ambient PM₂.₅. This study combined computed molecular properties with toxicologically relevant assay results to probe the OP of anthropogenically driven portions of ambient PM₂.₅, and results in a better understanding of the complexity of ambient PM₂.₅ OP.
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