Salt marsh estuaries serve as sources and sinks for nutrients and elements to and from estuarine water, which enhances and alleviates watershed fluxes to the coastal ocean. We assessed sources and sinks of mercury in the intertidal Plum Island Sound estuary in Massachusetts, the largest salt marsh estuary of New England, using 25-km spatial water sampling transects. Across all seasons, dissolved (FHg) and total (THg) mercury concentrations in estuarine water were highest and strongly enhanced in upper marshes (1.31 ± 0.20 ng L⁻¹ and 6.56 ± 3.70 ng L⁻¹, respectively), compared to riverine Hg concentrations (0.86 ± 0.17 ng L⁻¹ and 0.88 ± 0.34 ng L⁻¹, respectively). Mercury concentrations declined from upper to lower marshes and were lowest in ocean water (0.38 ± 0.10 ng L⁻¹ and 0.56 ± 0.25 ng L⁻¹, respectively). Conservative mixing models using river and ocean water as endmembers indicated that internal estuarine Hg sources strongly enhanced estuarine water Hg concentrations. For FHg, internal estuarine Hg contributions were estimated at 26 g yr⁻¹ which enhanced Hg loads from riverine sources to the ocean by 44%. For THg, internal sources amounted to 251 g yr⁻¹ and exceeded riverine sources six-fold. Proposed sources for internal estuarine mercury contributions include atmospheric deposition to the large estuarine surface area and sediment re-mobilization, although sediment Hg concentrations were low (average 23 ± 2 μg kg⁻¹) typical of uncontaminated sediments. Soil mercury concentrations under vegetation, however, were ten times higher (average 200 ± 225 μg kg⁻¹) than in intertidal sediments suggesting that high soil Hg accumulation might drive lateral export of Hg to the ocean. Spatial transects of methylated Hg (MeHg) showed no concentration enhancements in estuarine water and no indication of internal MeHg sources or formation. Initial mass balance considerations suggest that atmospheric deposition may either be in similar magnitude, or possibly exceed lateral tidal export which would be consistent with strong Hg accumulation observed in salt marsh soils sequestering Hg from current and past atmospheric deposition.

Fugitive emissions from natural gas systems are the largest anthropogenic source of the greenhouse gas methane (CH4) in the U.S. and contribute to the risk of explosions in urban environments. Here, we report on a survey of CH4 emissions from 100 natural gas leaks in cast iron distribution mains in Metro Boston, MA. Direct measures of CH4 flux from individual leaks ranged from 4.0 – 2.3 × 104 g CH4•day−1. The distribution of leak size is positively skewed, with 7% of leaks contributing 50% of total CH4 emissions measured. We identify parallels in the skewed distribution of leak size found in downstream systems with midstream and upstream stages of the gas process chain. Fixing ‘superemitter’ leaks will disproportionately stem greenhouse gas emissions. Fifteen percent of leaks surveyed qualified as potentially explosive (Grade 1), and we found no difference in CH4 flux between Grade 1 leaks and all remaining leaks surveyed (p = 0.24). All leaks must be addressed, as even small leaks cannot be disregarded as ‘safely leaking.’ Key methodological impediments to quantifying and addressing the impacts of leaking natural gas distribution infrastructure involve inconsistencies in the manner in which gas leaks are defined, detected, and classified. To address this need, we propose a two-part leak classification system that reflects both the safety and climatic impacts of natural gas leaks.

Urban vegetation is associated with numerous public health benefits; however, urban tree canopies may be threatened by fugitive methane exposure from leaky natural gas distribution systems. Despite anecdotal evidence of the harmful impacts of natural gas leaks on urban tree decline, the relationship between soil gas exposure and tree health has not been formally quantified in an urban setting. We conducted a case-control study to compare soil natural gas exposure in sidewalk tree pits of healthy and dead or dying trees in Chelsea, Massachusetts, during summer 2019. We measured soil concentrations of methane and oxygen at four points around the trunks of 84 case and 97 control trees. We determined that case trees had 30 times the odds of being exposed to detectable levels of soil methane relative to the control trees sampled (95% CI = 3.93, 229). Among tree pits with elevated soil gas, we also found that methane concentrations were highest on the side of the tree pit closest to the street. These results contribute evidence to support the widespread belief that soil methane exposure can negatively impact urban tree health. They also suggest that fugitive methane leakage from urban natural gas distribution systems beneath the street surface may be responsible for elevated soil gas concentrations in sidewalk tree pits and subsequent tree death.

On-road emissions vary widely on time scales as short as minutes and length scales as short as tens of meters. Detailed data on emissions at these scales are a prerequisite to accurately quantifying ambient pollution concentrations and identifying hotspots of human exposure within urban areas. We construct a highly resolved inventory of hourly fluxes of CO, NO2, NOx, PM2.5 and CO2 from road vehicles on 280,000 road segments in eastern Massachusetts for the year 2012. Our inventory integrates a large database of hourly vehicle speeds derived from mobile phone and vehicle GPS data with multiple regional datasets of vehicle flows, fleet characteristics, and local meteorology. We quantify the ‘excess’ emissions from traffic congestion, finding modest congestion enhancement (3–6%) at regional scales, but hundreds of local hotspots with highly elevated annual emissions (up to 75% for individual roadways in key corridors). Congestion-driven reductions in vehicle fuel economy necessitated ‘excess’ consumption of 113 million gallons of motor fuel, worth ∼ $415M, but this accounted for only 3.5% of the total fuel consumed in Massachusetts, as over 80% of vehicle travel occurs in uncongested conditions. Across our study domain, emissions are highly spatially concentrated, with 70% of pollution originating from only 10% of the roads. The 2011 EPA National Emissions Inventory (NEI) understates our aggregate emissions of NOx, PM2.5, and CO2 by 46%, 38%, and 18%, respectively. However, CO emissions agree within 5% for the two inventories, suggesting that the large biases in NOx and PM2.5 emissions arise from differences in estimates of diesel vehicle activity. By providing fine-scale information on local emission hotspots and regional emissions patterns, our inventory framework supports targeted traffic interventions, transparent benchmarking, and improvements in overall urban air quality.

Understanding the factors that affect spatial differences in PM2.5 composition is crucial for implementing emissions control and health policies. Although previous studies have explored modeling of spatial patterns as a tool to improve human exposure assessment, little work has employed a multivariate clustering approach to identify spatial patterns in particle composition. In this study, we used this approach to assess the spatial patterns of ambient PM2.5 elemental concentrations in Eastern Massachusetts in the United States. To distinguish one cluster of sites from another, we considered air pollution sources and geodemographic variables. We evaluated spatial patterns for 11 elemental components of ambient PM2.5, which included S, K, Ca, Fe, Zn, Cu, Ti, Al, Pb, V, and Ni. The analyses for S, Ca, Cu, Ti, Al, and Pb resulted in: 2 clusters for Fe, Zn, V, and Ni; 3 clusters; and for 12 clusters for K. Overall, our findings suggest substantial variation of clusters among PM2.5 components. In addition, land use, population density, and daily traffic were used as variables to more effectively characterize clusters of sites. We used R2 values to estimate the effectiveness of each variable in characterizing clusters. Larger R2 values indicate better the discrimination among the sites. For example, population density had the highest R2 value when the analysis was performed for S, Ca, Zn, Ti, Al, Pb, and V; land use presented the highest R2 value for Cu, V, and Ni; and, traffic showed the highest R2 value for PM2.5 mass concentration. This study improves the ability to model both the between- and within-area variability of source emissions and pollution regime, using concentrations of PM2.5 components.

Exposure to traffic-related PM₂.₅ mass and its components can affect human health. Meanwhile, indoor concentrations are better exposure predictors as compared to outdoor concentrations because individuals spend the majority of their time indoors. We estimated the impact of traffic emissions on indoor PM₂.₅ mass and its species as a function of road proximity in Massachusetts. A linear regression model was built using 662 indoor samples and 580 ambient samples. Analysis shows that indoor exposures to traffic-related particles increased dramatically with road proximity. We defined relative concentration decrease, R(α), as the ratio of the indoor concentration at perpendicular distance α in meters from the closest major road to the indoor concentration at 1800 m from the major road. R(13) values for PM₂.₅ mass and Black Carbon (BC) were 1.3 (95%CI: 1.4, 1.6) and 2.1 (95%CI: 1.3, 2.8) for A12 roads, and 1.3 (95%CI: 1.2, 1.4) and 1.2 (95%CI: 1.1, 1.3) for A3 roads. R(α) values were also estimated for Fe, Mn, Mo, Sr and Ti for A12 roads, and Ca, Cu, Fe, Mn, Mo, Ni, Si, Sr, V and Zn for A3 roads. R(α) values for species associated mainly with brakes, tires or road dust (e.g., Mn, Mo and Sr) were higher than others. For A12 roads, R(13) values for Mn and Mo were 10.9 (95%CI: 0.9, 20.9) and 6.5 (95%CI: 1.4, 11.5), and ranged from 1.3 to 2.1 for other species; for A3 roads, R(13) values for Mn, Mo and Sr were 1.9 (95%CI: 1.1, 2.9), 1.8 (95%CI: 1.1, 2.4), and 8.5 (95%CI: 5.9, 10.9), and ranged from 1.2 to 1.6 for others. Our results indicate a significant impact of local traffic emissions on indoor air, which depends on road proximity. Thus road proximity which has been used in many epidemiological studies is a reasonable exposure metric.

Physical dynamics of Harmful Algal Blooms in Massachusetts Bay in May 2005 and 2008 were examined by the simulated results. Reverse particle-tracking experiments suggest that the toxic phytoplankton mainly originated from the Bay of Fundy in 2005 and the western Maine coastal region and its local rivers in 2008. Mechanism studies suggest that the phytoplankton were advected by the Gulf of Maine Coastal Current (GMCC). In 2005, Nor'easters increased the cross-shelf surface elevation gradient over the northwestern shelf. This intensified the Eastern and Western MCC to form a strong along-shelf current from the Bay of Fundy to Massachusetts Bay. In 2008, both Eastern and Western MCC were established with a partial separation around Penobscot Bay before the outbreak of the bloom. The northeastward winds were too weak to cancel or reverse the cross-shelf sea surface gradient, so that the Western MCC carried the algae along the slope into Massachusetts Bay.

Spatial gradients of polychlorinated biphenyls (PCBs) and organochlorine pesticides were examined in the young-of-the-year (YOY) bluefish (Pomatomus saltatrix) in the vicinity of a PCB Superfund Site in New Bedford Harbor, Massachusetts, and in the adjacent waters. PCB concentrations in bluefish varied between different locations, and also among fish from a given location. A generally decreasing gradient in PCB concentrations was evident as the bluefish were collected away from the Superfund Site. The average sum of PCB concentrations were highest for bluefish collected in the Upper Harbor between Interstate-195 Bridge and Coggeshall Street Bridge (Upper Harbor), followed by bluefish in Lower Harbor from north of Popes Island Bridge (Lower Harbor), and bluefish from Outer Harbor south of Hurricane Barrier (Outer Harbor). The levels of PCBs in bluefish from Clarks Cove and PCBs in bluefish from Buzzards Bay were similar and lowest among all bluefish specimens analyzed in the present study. Pesticide concentrations were about one order of magnitude or lower than the PCB concentrations, and the gradient of pesticide concentrations generally followed the gradient of PCB concentrations. Some of the commonly detected pesticides in the order of decreasing concentrations included DDTs and metabolites, heptachlor epoxide, endosulfan sulfate, and α-chlordane. Distribution of PCBs and organochlorine pesticides were examined in the tissues of YOY bluefish from Clarks Cove. PCBs and lipids in the brain samples of YOY bluefish were generally numerically greater than PCBs in the liver samples, but these differences were not statistically significant. PCBs and lipids in hypaxial muscle samples were numerically greater than PCBs in epaxial muscle samples, although these two groups of tissues were not statistically different. Despite the higher susceptibility of lighter PCB homologs to geophysical and biogeochemical weathering processes, the relative dominance of lighter homologs in the Upper Harbor and Lower Harbor samples suggested ongoing or recent sources of these lighter PCBs, particularly Aroclor 1242 and Aroclor 1016 in this area. The presence of heavier homologs in the Upper Harbor and Lower Harbor bluefish samples could be attributed to Aroclor 1252 and Aroclor 1254 that were being used in relatively smaller quantities in the manufacture of electrical components in addition to Aroclor 1242 and Aroclor 1016. The concentration of heavier PCB homologs appears to increase in YOY bluefish the further away from the PCB Superfund Site in the Acushnet Estuary the samples were collected. Principal component analyses of PCB 153 normalized concentrations of the individual PCB congeners resulted in two general groupings; a relatively tight group comprised of YOY bluefish from Upper Harbor, Lower Harbor, and Outer Harbor, and a rather loose and more dispersed group comprised of Buzzards Bay bluefish and the tissue samples of bluefish from Clarks Cove. Principal component analyses of major pesticides suggested close groupings of bluefish from Clarks Cove and bluefish from Buzzards Bay. Pesticides in bluefish from Upper Harbor, Lower Harbor, and Outer Harbor formed a loose group, with some bluefish from these locations populating close to Clarks Cove and Buzzards Bay bluefish. Although PCBs have been implicated in various behavioral and health effects in the experimental and field studies, the deleterious effects of chronic exposure to high concentrations of PCBs and the potential for recruitment of New Bedford Harbor YOY bluefish population to the adult stock remains obscure. Adaptive or evolutionary resistance to contaminants have been documented in resident species in some highly contaminated estuaries, however similar responses have not been investigated in the migratory species like bluefish. The results of the present study provide a reference baseline for YOY bluefish for “before-and-after” comparative studies and other toxicological studies for the New Bedford Harbor Superfund Site that is currently being remediated.

Human activity and urbanization are having profound effects on natural landscapes and ecosystems. The presence and persistence of human-made materials such as microplastics can have major impacts on the health of organisms in both marine and terrestrial environments. We quantified microplastics in herring gull (Larus argentatus) and great black-backed gull (Larus marinus) nests at three colonies in the northeast United States that varied in their degree of urbanization: Jamaica Bay (JB) in New York City, Youngs Island (YI) on Long Island, New York, and Tuckernuck Island (TN) in Massachusetts. Nests in urban colonies contained a higher proportion of microplastics than those in the more remote colony. Our results link urbanization with microplastic accumulation in coastal environments and suggest that assessing microplastics in seabird nests could provide a means of evaluating microplastics encountered by seabirds and other coastal marine animals.