Recent studies indicate that PAH transformation products such as ketone or quinone-substituted PAHs (OPAHs) are potent aryl hydrocarbon receptor (AhR) activators that elicit toxicological effects independent of those observed for PAHs. Here, we measured eight OPAHs, two sulfur-containing (SPAH), one oxygen-containing (DBF), and one nitrogen-containing (CARB) heterocyclic PAHs (i.e. ΣONS-PAHs = OPAH8 + SPAH + DBF + CARB) in 35 stream sediments collected from a small (∼1303 km²) urban watershed located in south-central Pennsylvania, USA. Combined ΣONS-PAH concentrations ranged from 59 to 1897 μg kg⁻¹ (mean = 568 μg kg⁻¹; median = 425 μg kg⁻¹) and were 2.4 times higher in urban versus rural areas, suggesting that activities taking place on urban land serve as a source of ΣONS-PAHs to sediments. To evaluate urban land use metrics that might explain these data, Spearman rank correlation analyses was used to evaluate the degree of association between ΣONS-PAH concentrations and urban land-use/land-cover metrics along an urban-rural transect at two spatial scales (500-m and 1000-m upstream). Combined ΣONS-PAH concentrations showed highly significant (p < 0.0001) correlations with ΣPAH19, residential and commercial/industrial land use (RESCI), and combined state and local road miles (MILES), suggesting that ΣONS-PAHs originate from similar sources as PAHs. To evaluate OPAH sources, a subset of ΣONS-PAHs for which reference assemblages exist, an average OPAH fractional assemblage for urban sediments was derived using agglomerative hierarchal cluster (AHC) analysis, and compared to published OPAH source profiles. Urban sediments from the Condoguinet Creek (n = 21) showed highly significant correlations with urban particulate matter (X² = 0.05, r = 0.91, p = 0.0047), suggesting that urban particulate matter is an important OPAH source to sediments in this watershed. Results suggest the inclusion of ΣONS-PAH measurements adds value to traditional PAH analyses, and may help elucidate and refine pollutant source identification in urban watersheds.

Since the early 2000s, an increasing number of power plants in the U.S. have switched from burning coal to burning gas and thus have released less SO₂ emissions into the atmosphere. We investigated whether stream chemistry (i.e., SO₄²⁻) also benefits from this transition. Using publicly available data from Pennsylvania (PA), a U.S. state with heavy usage of coal as fuel, we found that the impact of SO₂ emissions on stream SO₄²⁻ can be observed as far as 63 km from power plants. We developed a novel model that incorporates an emission-control technology trend for coal-fired power plants to quantify potentially avoided SO₂ emissions and stream SO₄²⁻ as power plants switched from coal to gas. The results show that, if 30% of the electricity generated by coal in PA in 2017 had been replaced by that from natural gas, a total of 20.3 thousand tons of SO₂ emissions could have been avoided and stream SO₄²⁻ concentrations could have decreased as much as 10.4%. Extrapolating the model to other states in the U.S., we found that as much as 46.1 thousand tons of SO₂ emissions per state could have been avoided for a similar 30% coal-to-gas switch, with potential amelioration of water quality near power plants. The emission-control technology trend model provides a valuable tool for policy makers to assess the benefits of coal-to-gas shifts on water quality improvements as well as the effectiveness of emission control technologies.

At a 50-year-old coal mine drainage barrens in central Pennsylvania, USA, we evaluated the biogeochemistry of acidic, Fe(III)oxy(hydr)oxide precipitates in reclaimed plots and compared them to untreated precipitates in control areas. Reclaimed plots supported successional vegetation that became established after a one-time compost and lime treatment in 2006, while control plots supported biological crusts. Precipitates were sampled from moist yet unsaturated surface layers in an area with lateral subsurface flow of mine drainage above a fragipan. Fe(II) concentrations were three- to five-fold higher in reclaimed than control precipitates. Organically bound Fe and amorphous iron oxides, as fractions of total Fe, were also higher in reclaimed than control precipitates. Estimates of Fe-reducing and Fe-oxidizing bacteria were four- to tenfold higher in root-adherent than both types of control precipitates. By scaling up measurements from experimental plots, total Fe losses during the 5-yr following reclamation were estimated at 45 t Fe ha−1 yr−1.

Three sets of model predicted values for speciated mercury concentrations and dry deposition fluxes over the Great Lakes region were assessed using field measurements and model intercomparisons. The model predicted values were produced by the Community Multiscale Air Quality Modeling System for the year 2002 (CMAQ2002) and for the year 2005 (CMAQ2005) and by the Global/Regional Atmospheric Heavy Metals Model for the year 2005 (GRAHM2005). Median values of the surface layer ambient concentration of gaseous elemental mercury (GEM) from all three models were generally within 30% of measurements. However, all three models overpredicted surface-layer concentrations of gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) by a factor of 2–10 at the majority of the 15 monitoring locations. For dry deposition of GOM plus PBM, CMAQ2005 showed a clear gradient with the highest deposition in Pennsylvania and its surrounding areas while GRAHM2005 showed no such gradient in this region; however, GRAHM2005 had more hot spots than those of CMAQ2005. Predicted dry deposition of GOM plus PBM from these models should be treated as upper-end estimates over some land surfaces in this region based on the tendencies of all the models to overpredict GOM and PBM concentrations when compared to field measurements. Model predicted GEM dry deposition was found to be as important as GOM plus PBM dry deposition as a contributor to total dry deposition. Predicted total annual mercury dry deposition were mostly lower than 5 μg m⁻² to the surface of the Great lakes, between 5 and 15 μg m⁻² to the land surface north of the US/Canada border, and between 5 and 40 μg m⁻² to the land surface south of the US/Canada border. Predicted dry deposition from different models differed from each other by as much as a factor of 2 at regional scales and by a greater extent at local scales.

Mobile monitoring is an useful approach for measuring intra-urban variation of air pollution in urban environments. In this study, we used a mobile monitoring approach to study the spatial-temporal variability of air and noise pollution in urban neighborhoods of Philadelphia. During summer 2017, we used portable instruments to measure PM2.5, black carbon (BC), and noise levels along 5 km paths in four residential neighborhoods (Tioga, Mill Creek, Chestnut Hill, and Northern Liberties) and one commercial district (Center City) in Philadelphia, Pennsylvania, USA. A total of 62 sets of measurements were made at three different times of day (during morning rush hour, mid-afternoon, and during afternoon rush hour) from June 5 to July 7, 2017. Spatially, there was a significant difference in PM2.5 concentrations among the four residential neighborhoods. Overall, the Chestnut Hill neighborhood had the highest PM2.5 concentrations (13.25 ± 6.89 μg/m3), followed by Tioga (9.58 ± 4.83 μg/m3), Northern Liberties (7.02 ± 4.17 μg/m3), and Mill Creek (3.9 ± 4.5 μg/m3). There was temporal variability of pollutants depending on the neighborhood; Northern Liberties demonstrated the highest temporal variability in these data. The highest PM2.5 (18.86 ± 3.17 μg/m3) was measured in the Chestnut Hill neighborhood during morning rush hour. Mean PM2.5, BC, and noise levels based on mobile measurements at Philadelphia during summer 2017 were 8.41 ± 4.31 μg/m3, 0.99 ± 0.44 μg C/m3, and 62.01 ± 3.20 dBA, respectively. Environmental noise showed the highest temporal variation of the monitored components for 3 time periods. Generally, an increase in tree cover led to a decrease in PM2.5.

We used land-use analysis, PAH concentrations and assemblages, and multivariate statistics to identify sediment PAH sources in a small (∼1303 km2) urbanizing watershed located in South-Central, Pennsylvania, USA. A geographic information system (GIS) was employed to quantify land-use features that may serve as PAH sources. Urban PAH concentrations were three times higher than rural levels, and were significantly and highly correlated with combined residential/commercial/industrial land use. Principal components analysis (PCA) was used to group sediments with similar PAH assemblages, and correlation analysis compared PAH sediment assemblages to common PAH sources. The strongest correlations were observed between rural sediments (n = 7) and coke-oven emissions sources (r = 0.69–0.78, n = 5), and between urban sediments (n = 22) and coal-tar-based sealcoat dust (r = 0.94, n = 47) suggesting that coal-tar-based sealcoat is an important urban PAH source in this watershed linked to residential and commercial/industrial land use.

Historic emissions from two zinc smelters have injured the forest on Blue Mountain near Palmerton, Pennsylvania, USA. Seedlings of soybeans and five tree species were grown in a greenhouse in a series of mixtures of smelter-contaminated and reference soils and then phytotoxic thresholds were calculated. As little as 10% Palmerton soil mixed with reference soil killed or greatly stunted seedlings of most species. Zinc was the principal cause of the phytotoxicity to the tree seedlings, although Mn and Cd may also have been phytotoxic in the most contaminated soil mixtures. Calcium deficiency seemed to play a role in the observed phytotoxicity. Exposed soybeans showed symptoms of Mn toxicity. A test of the effect of liming on remediation of the Zn and Mn phytotoxicity caused a striking decrease in Sr-nitrate extractable metals in soils and demonstrated that liming was critical to remediation and restoration.