Isotopic Signatures and Outputs of Lead from Coal Fly Ash Disposal in China, India, and the United States.

Despite extensive research and technology to reduce the atmospheric emission of Pb from burning coal for power generation, minimal attention has been paid to Pb associated with coal ash disposal in the environment. This study investigates the isotopic signatures and output rates of Pb in fly ash disposal in China, India, and the United States. Pairwise comparison between feed coal and fly ash samples collected from coal-fired power plants from each country shows that the Pb isotope composition of fly ash largely resembles that of feed coal, and its isotopic distinction allows for tracing the release of Pb from coal fly ash into the environment. Between 2000 and 2020, approx. 236, 56, and 46 Gg Pb from fly ash have been disposed in China, India, and the U.S., respectively, posing a significant environmental burden. A Bayesian Pb isotope mixing model shows that during the past 40 to 70 years, coal fly ash has contributed significantly higher Pb (∼26%) than leaded gasoline (∼7%) to Pb accumulation in the sediments of five freshwater lakes in North Carolina, U.S.A. This implies that the release of disposed coal fly ash Pb at local and regional scales can outweigh that of other anthropogenic Pb sources.

Positive outcomes from U.S. lead regulations, continued challenges, and lessons learned for regulating emerging contaminants.

Albeit slow and not without its challenges, lead (Pb) emissions and sources in the United States (U.S.) have decreased immensely over the past several decades. Despite the prevalence of childhood Pb poisoning throughout the twentieth century, most U.S. children born in the last two decades are significantly better off than their predecessors in regard to Pb exposure. However, this is not equal across demographic groups and challenges remain. Modern atmospheric emissions of Pb in the U.S. are nearly negligible since the banning of leaded gasoline in vehicles and regulatory controls on Pb smelting plants and refineries. This is evident in the rapid decrease of atmospheric Pb concentrations across the U.S. over the last four decades. One of the most significant remaining contributors to air Pb is aviation gasoline (avgas), which is minor compared to former Pb emissions. However, continual exposure risks to Pb exist in older homes and urban centers, where leaded paint and/or historically contaminated soils + dusts can still harm children. Thus, while effective in eliminating nearly all primary sources of Pb in the environment, the slow rate of U.S. Pb regulation has led to legacy sources of Pb in the environment. More proactive planning, communication, and research of commonly used emerging contaminants of concern that can persist in the environment long after their initial use (i.e., PFAS) should be prioritized so that the same mistakes are not made again.

Predictive modeling of indoor dust lead concentrations: Sources, risks, and benefits of intervention.

Lead (Pb) contamination continues to contribute to world-wide morbidity in all countries, particularly low- and middle-income countries. Despite its continued widespread adverse effects on global populations, particularly children, accurate prediction of elevated household dust Pb and the potential implications of simple, low-cost household interventions at national and global scales have been lacking. A global dataset (∼40 countries, n = 1951) of community sourced household dust samples were used to predict whether indoor dust was elevated in Pb, expanding on recent work in the United States (U.S.). Binned housing age category alone was a significant (p < 0.01) predictor of elevated dust Pb, but only generated effective predictive accuracy for England and Australia (sensitivity of ∼80%), similar to previous results in the U.S. This likely reflects comparable Pb pollution legacies between these three countries, particularly with residential Pb paint. The heterogeneity associated with Pb pollution at a global scale complicates the predictive accuracy of our model, which is lower for countries outside England, the U.S., and Australia. This is likely due to differing environmental Pb regulations, sources, and the paucity of dust samples available outside of these three countries. In England, the U.S., and Australia, simple, low-cost household intervention strategies such as vacuuming and wet mopping could conservatively save 70 billion USD within a four-year period based on our model. Globally, up to 1.68 trillion USD could be saved with improved predictive modeling and primary intervention to reduce harmful exposure to Pb dust sources.

Using community science for detailed pollution research: a case-study approach in Indianapolis, IN, USA.

Heavy metal contamination in urban environments, particularly lead (Pb) pollution, is a health hazard both to humans and ecological systems. Despite wide recognition of urban metal pollution in many cities, there is still relatively limited research regarding heavy metal distribution and transport at the household-scale between soils and indoor dusts-the most important scale for actual human interaction and exposure. Thus, using community-scientist-generated samples in Indianapolis, IN (USA), we applied bulk chemistry, Pb isotopes, and scanning electron microscopy (SEM) to illustrate how detailed analytical techniques can aid in interpretation of Pb pollution distribution at the household-scale. Our techniques provide definitive evidence for Pb paint sourcing in some homes, while others may be polluted with Pb from past industrial/vehicular sources. SEM revealed anthropogenic particles suggestive of Pb paint and the widespread occurrence of Fe-rich metal anthropogenic spherules across all homes, indicative of pollutant transport processes. The variability of Pb pollution at the household scale evident in just four homes is a testament to the heterogeneity and complexity of urban pollution. Future urban pollution research efforts would do well to utilize these more detailed analytical methods on community-sourced samples to gain better insight into where the Pb came from and how it currently exists in the environment. However, these methods should be applied after large-scale pollution screening techniques such as portable X-ray fluorescence (XRF), with more detailed analytical techniques focused on areas where bulk chemistry alone cannot pinpoint dominant pollution mechanisms and where community scientists can also give important metadata to support geochemical interpretations.

Rural and Urban Ecologies of Early Childhood Toxic Lead Exposure: The State of Kansas, 2005 to 2012.

Introduction: No safe detectable level of lead (Pb) exists in the blood of children. Until recently, U.S. Centers for Disease Control and Prevention (CDC) guidelines designated a blood lead level (BLL) ≥ 5 µg/dL as an elevated BLL (EBLL). For the State of Kansas, early childhood blood lead burdens lack reporting in the literature. Methods: Secondary analysis was conducted of passively reported EBLL rates ≥ 5 µg/dL among children ages 0 - 5 years at the zip code-level in Kansas during 2005 to 2012. Data weights using corresponding population estimates were applied to produce statewide outcomes. Results: Statewide estimates of annual testing coverage in Kansas among children ages 0 - 5 years were low (9.7%). Approximately 17,000 children ages 0 - 5 years developed an EBLL ≥ 5 µg/dL each year in Kansas with a 6.9% statewide EBLL rate compared to the national rate of 3.2% for the corresponding years. Significant variations in EBLL rates were found between suburban zip codes compared to urban, urban cluster, or rural at 3.1%, 7.2%, 8.8%, and 10.0%, respectively. Among the worst outcomes in EBLL rates was observed for zip codes in southeast Kansas (13.5%) and rural areas with < 500 persons (15.1%). Conclusions: Young children in Kansas had twice the risk of developing an EBLL ≥ 5 µg/dL compared to the national rate, while higher rates consistently were seen outside of the suburbs and particularly in more rural and less populated areas. At-risk children and troubled areas of toxic lead exposure in the State of Kansas require increased recognition with improved targeting and interventions.

Using Community Science to Better Understand Lead Exposure Risks.

Lead (Pb) is a neurotoxicant that particularly harms young children. Urban environments are often plagued with elevated Pb in soils and dusts, posing a health exposure risk from inhalation and ingestion of these contaminated media. Thus, a better understanding of where to prioritize risk screening and intervention is paramount from a public health perspective. We have synthesized a large national data set of Pb concentrations in household dusts from across the United States (U.S.), part of a community science initiative called "DustSafe." Using these results, we have developed a straightforward logistic regression model that correctly predicts whether Pb is elevated (>80 ppm) or low (<80 ppm) in household dusts 75% of the time. Additionally, our model estimated 18% false negatives for elevated Pb, displaying that there was a low probability of elevated Pb in homes being misclassified. Our model uses only variables of approximate housing age and whether there is peeling paint in the interior of the home, illustrating how a simple and successful Pb predictive model can be generated if researchers ask the right screening questions. Scanning electron microscopy supports a common presence of Pb paint in several dust samples with elevated bulk Pb concentrations, which explains the predictive power of housing age and peeling paint in the model. This model was also implemented into an interactive mobile app that aims to increase community-wide participation with Pb household screening. The app will hopefully provide greater awareness of Pb risks and a highly efficient way to begin mitigation.

Road sediment, an underutilized material in environmental science research: A review of perspectives on United States studies with international context.

Road sediment is a pervasive environmental medium that acts as both source and sink for a variety of natural and anthropogenic particles and often is enriched in heavy metals. Road sediment is generally understudied in the United States (U.S.) relative to other environmental media and compared to countries such as China and the United Kingdom (U.K.). However, the U.S. is an ideal target for these studies due to the diverse climates and wealth of geochemical, socioeconomic, demographic, and health data. This review outlines the existing U.S. road sediment literature while also providing key international perspectives and context. Furthermore, the most comprehensive table of U.S. road sediment studies to date is presented, which includes elemental concentrations, sample size, size fraction, collection and analytical methods, as well as digestion procedure. Overall, there were observed differences in studies by sampling time period for elemental concentrations, but not necessarily by climate in the U.S. Other key concepts addressed in this road sediment review include the processes controlling its distribution, the variety of nomenclature used, anthropogenic enrichment of heavy metals, electron microscopy, health risk assessments, remediation, and future directions of road sediment investigations. Going forward, it is recommended that studies with a higher geographic diversity are performed that consider smaller cities and rural areas. Furthermore, environmental justice must be a focus as community science studies of road sediment can elucidate pollution issues impacting areas of high need. Finally, this review calls for consistency in sampling, data reporting, and nomenclature to effectively expand work on understudied elements, particles, and background sediments.

Quantification of Pb pollution sources in complex urban environments through a multi-source isotope mixing model based on Pb isotopes in lichens and road sediment.

Despite a growing focus on anthropogenic toxic metal pollution in urban environments, few studies have addressed the problem of quantification when more than two pollution sources are likely present, particularly within complex urban settings in the United States (U.S.). In this study, we utilize the MixSIAR package in R for source apportionment based on Pb isotopic signatures in lichen and road sediment in two urban-industrial centers in SW Ohio (OH). We show that ranges of pollutant contributions are more useful than only visualizing mean or raw values of source apportionment, because this avoids overinterpretation of data when certain sources have a large range of uncertainty. We point out both the dominance of industrial pollution as well as the legacy of leaded gasoline pollution in typical mid-sized U.S. cities, which is evident in both road sediment and lichens. Leaded gasoline contribution to Pb in Middletown, OH lichens mostly vary between ~10 and 25%, while in Hamilton, OH the contribution to lichens and road sediment tends to be relatively negligible except for two road sediment samples and one lichen sample, where median contributions are ~20-30%. Industrial combustion pollution source contributions vary between ~25 and 75% in Hamilton, and ~50-100% in Middletown, OH. Furthermore, comparing pollution sources in lichens to modern particulate matter can provide a record of how pollutant sources change over time, such as our traffic lichen (Sample Li-9) plotting closer to leaded gasoline on a bivariate mixing diagram than modern traffic particulate matter, or our coke plant lichen containing slightly less Pb contribution from industrial combustion sources relative to modern coke plant particulate matter. Lastly, when applicable, multi-source mixing models should be complimented in future studies with additional isotopic source tracers such as Cu, Zn, Nd, and Os to further elucidate unique sources of metal pollutants in addition to Pb.

Influences on tidal channel and aquaculture shrimp pond water chemical composition in Southwest Bangladesh.

Detailed geochemical studies of both major and minor elements in Bangladesh surface waters are sparse, particularly in shrimp aquaculture pond environments. Therefore, water samples from shrimp aquaculture ponds and tidal channels were collected in high precipitation (July) and low precipitation (May) months from 2018-2019 in Southwest Bangladesh and analyzed for complete water chemistry. Selenium (Se) and arsenic (As) were elevated above WHO guidelines in 50% and ~ 87% of samples, respectively, but do not show any recognizable spatial patterns. Shrimp pond and tidal channel water compositions in the dry season (May) are similar, illustrating their connectivity and minimal endogenous effects within shrimp ponds. Tidal channels are less saline in July than shrimp ponds still irrigated by tidal channels, suggesting that either farmers limit irrigation to continue farming saltwater shrimp, or the irrigation flux is low and leads to a lag in aquaculture-tidal channel compositional homogenization. δ18O and δ2H isotopic compositions from samples in May of 2019 reveal tidal channel samples are closer to the local meteoric water line (LMWL) than shrimp pond samples, because of less evaporation. However, evaporation in May shrimp ponds has a minimal effect on water composition, likely because of regular drainage/exchange of pond waters. Dissolved organic carbon (DOC) is positively correlated with both δ18O and δ2H in shrimp ponds, suggesting that as evaporation increases, DOC becomes enriched. Multiple linear regression reveals that As and Se can be moderately predicted (adjusted R2 values between 0.4 and 0.7, p < 0.01) in surface waters of our study with only 3-4 independent predictor variables (e.g., Ni, V and DOC for Se prediction; Cu, V, Ni and P for As prediction). Thus, this general approach should be followed in other regions throughout the world when measurements for certain hazardous trace elements such as Se and As may be lacking in several samples from a dataset.

Geochemical partitioning and possible heavy metal(loid) bioaccumulation within aquaculture shrimp ponds.

Limited work has been conducted on trace metal(loid) exchange between sediment, water, feed, and shrimp, particularly in estuarine aquaculture environments. To identify metal(loid) sources and the processes controlling bioaccumulation in shrimp, we analyzed paired aquaculture water, sediment, and shrimp samples collected in Southwest Bangladesh in the late dry season (May), as well as several common artificial feeds. Additionally, we analyzed sediment extract samples from 24-hour laboratory batch experiments as an analogue for aquaculture pond sediment porewater to examine element mobilization from pond sediment. Weak correlations between element concentrations in extracts, pond water, and bulk sediment indicate equilibrium with sediment was not achieved in extract experiments or ponds, and that sediment composition has little influence on pond water or shrimp composition. Aquaculture shrimp metal(loid) concentrations were similar to artificial feed but not pond sediment or pond water, suggesting that shrimp composition is mostly influenced by diet. Although arsenic (As) and selenium (Se) were present at high concentrations in shrimp pond waters and sediment, they were often below detection in shrimp. However, the highly toxic metal thallium (Tl) was detected in shrimp at levels that pose significant human health risks based on calculated target hazard quotient (THQ) values. Thus, further research into potential Tl contamination in Bangladesh aquaculture environments is warranted.

A first-order geochemical budget for suspended sediment discharge to the Bay of Bengal from the Ganges-Brahmaputra river system.

The Ganges-Brahmaputra-Meghna (G-B) river system transports >1 × 109 t/yr of sediment, with an estimated 0.7 × 109 t/yr reaching the Bay of Bengal (BoB). This discharge represents a major input of sediment and associated elements to the global ocean, but quantification of the sediment-element mass reaching the BoB has yet to be fully explored. Published geochemical and suspended sediment data are used to calculate a first-order budget for the modern sediment supply of geochemical elements to the BoB. River profile bulk sediment-element concentrations are calculated based on suspended sediment and element measurements taken in the Ganges and Brahmaputra rivers. A Monte Carlo analysis is applied to account for variable sediment and geochemical contributions from each river. Results show that on average, the G-B system contributes ~5% of the global riverine discharge of solid-phase elements from sediment to the oceans. G-B sediments transport >10% of the global element supply of Hf and Zr. For others, like As and Cu, contributions from the G-B are <5%. Results also show that sediment reaching the BoB is relatively enriched in Hf, Zr, Th, REEs, Sn, and Bi, and majorly depleted in Na and Sr compared to UCC elemental concentrations. While limited by data availability and necessary simplifying assumptions, this study nevertheless provides a reasonable first-order budget for the modern discharge of solid-phase elements to the BoB. Insights from this work are significant for understanding the role of the G-B river system in global elemental cycling, and for providing a basis of comparison for future sediment-element discharge in light of rapid environmental change taking place in the region.

The first pollution investigation of road sediment in Gary, Indiana: Anthropogenic metals and possible health implications for a socioeconomically disadvantaged area.

An investigation of road sediment in Gary, Indiana revealed high levels of various trace metals such as Zn, Mn, and Cr, often exceeding those of background reference concentrations as shown through geoaccumulation indices and contamination factors. The hazard index (HI) value for Mn in children was >1 (1.7), suggesting possible long-term non-carcinogenic health risk. Mn HI for children is even higher for the five samples closest to a US Steel facility, with an HI of 2.8. Through SEM-EDS analysis, the prevalence of small particulates (PM2.5 and PM2.5-10) containing potentially harmful elements such as Mn and Pb illustrate a health risk through direct inhalation or ingestion. The small nature of particulates in general may also pose an increased health risk for respiratory diseases such as asthma. Mn concentrations in the road sediment were particularly high, with 30 out of 32 samples exceeding 1800 ppm. Mn and V concentrations show a strong spatial trend of decreasing concentration away from a US Steel facility. These spatial trends along with correlation plots of the bulk chemistry suggest that industrial steel manufacturing, particularly US Steel in Gary, is a major contributing source of Mn and V. Fe and Cr show a moderate decrease in concentrations away from the US Steel facility, which suggests some sourcing from the steel facility when coupled with bulk chemistry plots. Zn and Cu do not show much evidence of sourcing from the US Steel facility, likely due to increased mixing from other sources. Further work constraining anthropogenic sources, the bioaccessible fraction of metals, and analysis of direct atmospheric particulates can help with remedial activity and risk assessment.

Metal pollution investigation of Goldman Park, Middletown Ohio: Evidence for steel and coal pollution in a high child use setting.

A geochemical investigation of both ballfield sediment and street sediment in a park adjacent to a major steel manufacturing site in Middletown, Ohio revealed Pb, Cu, Cr and Zn exceeded background levels, but in heterogeneous ways and in varying levels of health concern. Pb, Sn, and Zn had geoaccumulation values>2 (moderate to heavy pollutants) in street sediment samples. Cr had a geoaccumulation value>1, while Ni, W, Fe and Mn had geoaccumulation values between 1 and 0 in street sediment. Street sediment contamination factors for respective elements are Zn (10.41), Sn (5.45), Pb (4.70), Sb (3.45), Cr (3.19), W (2.59), and Mn (2.43). The notable elements with the highest factors for ball fields are Zn (1.72), Pb (1.36), Cr (0.99), V (0.95), and Mn (1.00). High correlation coefficients of known constituents of steel, such as Fe and Mo, Ni and Cr, W and Co, W and V, as well as particulate steel and coal spherule fragments found by SEM suggest probable sourcing of some of the metals from the AK Steel facility directly adjacent to the park. However, overall extensive heterogeneity of metal pollutants in the area points to the difficulties in sourcing pollutant metals, with many outside sources likely contributing as well. This study demonstrates that different sediment media can be impacted by significantly different metal pollutants even when in very close proximity to a single source and points to unrecognized complexity in urban pollution processes in the region. This study pertains to large-scale regional importance, as Middletown, Ohio is indicative of a typical post-industrial Midwestern U.S. city where limited investigation has been conducted regarding urban pollution and sourcing of materials.

In vitro canal and isthmus debris removal of the self-adjusting file, K3, and WaveOne files in the mesial root of human mandibular molars.

INTRODUCTION: The purpose of this study was to compare the effectiveness of debris removal between the Self-Adjusting File (SAF), WaveOne, and K3 file systems in the mesial roots of mandibular molars. In addition, the SAF was tested as a potential adjunct after instrumentation with other systems. METHODS: The mesial roots of 30 extracted mandibular molars were mounted in resin by using the K-Kube, sectioned at 2 and 4 mm from working length, and randomly placed into 3 groups: K3 group, sequential preparation with K3 files to an apical size of 35/.04; WaveOne group, preparation with WaveOne primary file; and SAF group, preparation with SAF. Images were taken before instrumentation, after instrumentation, after final irrigation, and after SAF adjunct irrigation. A cleanliness percentage was calculated by using interactive software. Comparisons between groups were analyzed with repeated-measures analysis of variance and post hoc tests (P < .05). RESULTS: There was no significant difference in canal cleanliness among the groups, but the WaveOne was significantly worse for isthmus cleanliness. Use of the SAF as an adjunct only significantly improved canal cleanliness in the K3 group at the 2-mm level by an average of 1.7%. CONCLUSIONS: There was no difference in canal cleanliness between the 3 file systems; however, the SAF and K3 files performed significantly better than the WaveOne with respect to isthmus cleanliness. When used as a final irrigation adjunct device after instrumentation, the SAF provided a significant improvement only in a subset of the K3 group.