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GeoHealth as a research paradigm offers the opportunity to re-evaluate common research engagement models and science training practices. GeoHealth challenges are often wicked problems that require both transdisciplinary approaches and the establishment of intimate and long-term partnerships with a range of community members. We examine four common modes of community engagement and explore how research projects are launched, who has the power in these relationships, and how projects evolve to become truly transformative for everyone involved., Competing Interests: The authors declare no conflicts of interest relevant to this study., (© 2021 The Authors. GeoHealth published by Wiley Periodicals LLC on behalf of American Geophysical Union.)

While the presence of legacy lead (Pb) in urban soil is well documented, less is known about the bioaccessibility, transport, and exposure pathways of urban soil Pb. We study Pb bioaccessibility in Roxbury and Dorchester, MA, urban gardens to assess exposure risk and identify remediation strategies, applicable locally and in urban gardens across the country. We work in partnership with The Food Project, which brings the goals and perspectives of local farmers to the center of the research process and enables efficient local application of results to reduce Pb exposure. We measure changes in Pb bioaccessibility as a function of growing material, grain size, and Pb source. In comparison to soils, compost has lower total Pb concentrations, has lower Pb solubility in gastric fluid, and limits fine particle resuspension. The mean bioaccessible Pb concentration of compost is 265 mg/kg, nearly an order of magnitude lower than that of soils, and compost contains 14% higher carbon content than soils, which may account for the observed 19% lower Pb bioaccessibility in compost. For all matrices (soil, raised bed fill, and compost) grain sizes <37 μm contain a disproportionate fraction of the total pool of bioaccessible Pb. Furthermore, the isotopic composition of Pb in the size fractions linked with resuspension and elevated blood lead levels is indicative of leaded gasoline and leaded paint even decades removed from the primary deposition of these sources., Competing Interests: The authors declare no conflicts of interest relevant to this study., (©2017. The Authors.)

Heavy metal contamination of surface waters at mining sites often involves complex interactions of multiple sources and varying biogeochemical conditions. We compared surface and subsurface metal loading from mine waste pile runoff and mine drainage discharge and characterized the influence of iron oxides on metal fate along a 0.9-km stretch of Tar Creek (Oklahoma, USA), which drains an abandoned Zn/Pb mining area. The importance of each source varied by metal; mine waste pile runoff contributed 70% of Cd, while mine drainage contributed 90% of Pb, and both sources contributed similarly to Zn loading. Subsurface inputs accounted for 40% of flow and 40-70% of metal loading along this stretch. Streambed iron oxide aggregate material contained highly elevated Zn (up to 27,000 μg g(-1)), Pb (up to 550 μg g(-1)) and Cd (up to 200 μg g(-1)) and was characterized as a heterogeneous mixture of iron oxides, fine-grain mine waste, and organic material. Sequential extractions confirmed preferential sequestration of Pb by iron oxides, as well as substantial concentrations of Zn and Cd in iron oxide fractions, with additional accumulation of Zn, Pb, and Cd during downstream transport. Comparisons with historical data show that while metal concentrations in mine drainage have decreased by more than an order of magnitude in recent decades, the chemical composition of mine waste pile runoff has remained relatively constant, indicating less attenuation and increased relative importance of pile runoff. These results highlight the importance of monitoring temporal changes at contaminated sites associated with evolving speciation and simultaneously addressing surface and subsurface contamination from both mine waste piles and mine drainage., (Copyright © 2014 The Authors. Published by Elsevier B.V. All rights reserved.)

Background: Significant lead poisoning has been associated with imported nonpaint products., Objectives: To describe cases of pediatric lead intoxication from imported Indian spices and cultural powders, determine lead concentrations in these products, and predict effects of ingestion on pediatric blood lead levels (BLLs)., Patients and Methods: Cases and case-study information were obtained from patients followed by the Pediatric Environmental Health Center (Children's Hospital Boston). Imported spices (n = 86) and cultural powders (n = 71) were analyzed for lead by using x-ray fluorescence spectroscopy. The simple bioaccessibility extraction test was used to estimate oral bioavailability. The integrated exposure uptake biokinetic model for lead in children was used to predict population-wide geometric mean BLLs and the probability of elevated BLLs (>10 microg/dL)., Results: Four cases of pediatric lead poisoning from Indian spices or cultural powders are described. Twenty-two of 86 spices and foodstuff products contained >1 microg/g lead (for these 22 samples, mean: 2.6 microg/g [95% confidence interval: 1.9-3.3]; maximum: 7.6 microg/g). Forty-six of 71 cultural products contained >1 microg/g lead (for 43 of these samples, mean: 8.0 microg/g [95% confidence interval: 5.2-10.8]; maximum: 41.4 microg/g). Three sindoor products contained >47% lead. With a fixed ingestion of 5 microg/day and 50% bioavailability, predicted geometric mean BLLs for children aged 0 to 4 years increased from 3.2 to 4.1 microg/dL, and predicted prevalence of children with a BLL of >10 microg/dL increased more than threefold (0.8%-2.8%)., Conclusions: Chronic exposure to spices and cultural powders may cause elevated BLLs. A majority of cultural products contained >1 microg/g lead, and some sindoor contained extremely high bioaccessible lead levels. Clinicians should routinely screen for exposure to these products.

Environmental lead contamination is prevalent in urban areas where soil represents a significant sink and pathway of exposure. This study characterizes the speciation of lead that is relevant to local recontamination and to human exposure in the backyard gardens of Roxbury and Dorchester, MA, USA. One hundred forty-one backyard gardens were tested by X-ray fluorescence, and 81% of gardens have lead levels above the US EPA action limit of 400 microg/g. Raised gardening beds are the in situ exposure reduction method used in the communities to promote urban gardening. Raised beds were tested for lead and the results showed that the lead concentration increased from an initial range of 150+/-40 microg/g to an average of 336 microg/g over 4 years. The percent distribution of lead in the fine grain soil (<100 microm) and the trace metal signature of the raised beds support the conclusion that the mechanism of recontamination is wind-transported particles. Scanning electron microscopy and sequential extraction were used to characterize the speciation of lead, and the trace metal signature of the fine grain soil in both gardens and raised gardening beds is characteristic of lead-based paint. This study demonstrates that raised beds are a limited exposure reduction method and require maintenance to achieve exposure reduction goals. An exposure model was developed based on a suite of parameters that combine relevant values from the literature with site-specific quantification of exposure pathways. This model suggests that consumption of homegrown produce accounts for only 3% of children's daily exposure of lead while ingestion of fine grained soil (<100 microm) accounts for 82% of the daily exposure. This study indicates that urban lead remediation on a yard-by-yard scale requires constant maintenance and that remediation may need to occur on a neighborhood-wide scale.

We characterized the lability and bioaccessibility of Zn, Pb, and Cd in size-fractionated mine waste at the Tar Creek Superfund Site (Oklahoma) to assess the potential for metal transport, exposure, and subsequent bioavailability. Bulk mine waste samples contained elevated Zn (9100 +/- 2500 ppm), Pb (650 +/- 360 ppm), and Cd (42 +/- 10 ppm), while particles with the greatest potential for windborne transport and inhalation (< 10 microm) contained substantially higher concentrations, up to 220 000 ppm Zn, 16 000 ppm Pb, and 530 ppm Cd in particles < 1 microm. Although the mined ore at Tar Creek primarily consisted of refractory metal sulfides with low bioavailability, sequential extractions and physiologically based extractions indicate that physical and chemical weathering have shifted metals into relatively labile and bioaccessible mineral phases. In < 37 microm mine waste particles, 50-65% of Zn, Pb, and Cd were present in the "exchangeable" and "carbonate" sequential extraction fractions, and 60-80% of Zn, Pb, and Cd were mobilized in synthetic gastric fluid, while ZnS and PbS exhibited minimal solubility in these solutions. Our results demonstrate the importance of site-specific characterization of size-fractionated contemporary mine waste when assessing the lability and bioavailability of metals at mine-waste impacted sites.

The chemistry of Pb in urban soil must be understood in order to limit human exposure to Pb in soil and produce and to implement remediation schemes. In inner-city gardens where Pb contamination is prevalent and financial resources are limited, it is critical to identify the variables that control Pb bioavailability. Field-portable X-ray fluorescence was used to measure Pb in 103 urban gardens in Roxbury and Dorchester, MA, and 88% were found to contain Pb above the USEPA reportable limit of 400 mug g(-1). Phosphorus, iron, loss on ignition, and pH data were collected, Pb-bearing phases were identified by X-ray diffraction, and Pb isotopes were measured using inductively coupled plasma mass spectrometry. Four test crops were grown both in situ and in Roxbury soil in a greenhouse, and plant tissue was analyzed for Pb uptake by polarized energy-dispersive X-ray fluorescence. Variation at the neighborhood scale in soil mineralogical and chemical characteristics suggests that the bioavailable fraction of Pb in gardens is site specific. Based on Pb isotope analysis, two historical Pb sources appear to dominate the inventory of Pb in Roxbury gardens: leaded gasoline ((207) Pb/(206) Pb = 0.827) and Pb-based paint ((207)Pb/(206) Pb = 0.867). Nearly 70% of the samples analyzed can be isotopically described by mixing these two end members, with Pb-based paint contributing 40 to 80% of the mass balance. A simplified urban human exposure model suggests that the consumption of produce from urban gardens is equivalent to approximately 10 to 25% of children's daily exposure from tap water. Furthermore, analysis of over 60 samples of plant tissue from the four test species suggests that in these urban gardens unamended phytoremediation is an inadequate tool for decreasing soil Pb.

Typha latifolia (cattail) sequesters arsenic within predominantlyferric iron root coatings, thus decreasing mobility of this toxic element in wetland sediments. Element-specific XRF microtomographic imaging illustrated a high spatial correlation between iron and arsenic in root plaques, with little arsenic in the interior of the roots. XANES analyses demonstrated that the plaque was predominantly ferric iron and contained approximately 20% As(III) and 80% As(V), which is significant because the two oxidation states form species that differ in toxicity and mobility. For the first time, spatial distribution maps of As oxidation states were developed, indicating that As(III) and As(V) are both fairly heterogeneous throughoutthe plaque. Chemical extractions showed that As was strongly adsorbed in the plaque rather than coprecipitated. Iron and arsenic concentrations ranged from 0.03 to 0.8 g Fe g(-1) wet plaque and 30 to 1200 microg As g(-1) wet plaque, consistent with a mechanism of As adsorption onto Fe(III) oxyhydroxide plaque. Because this mechanism decreases the concentrations of both As(III) and As(V) in groundwater, we propose that disruption of vegetation could increase the concentrations of mobile arsenic.

Human activities in urban areas can lead to both chemical pollution and physical alteration of stream habitats. The evaluation of ecological impacts on urban streams can be problematic where both types of degradation occur. Effects of contaminants, for example, may be masked if stream channelization, loss of riparian vegetation, or other physical stressors exert comparable or larger influences. In the Aberjona watershed (near Boston, MA, USA), we used physical, chemical, and biological indices to discern the relative impacts of physical and chemical stressors. We used standard protocols for assessing the biological condition of low-gradient streams, sampling macroinvertebrate communities from several different habitat types (e.g., overhanging bank vegetation, undercut bank roots, and vegetation on rocks). We strengthened the linkage between chemical exposure and macroinvertebrate response by measuring metal concentrations not only in sediments from the stream bottom but also in the vegetative habitats where the macroinvertebrates were sampled. Linear regression analysis indicated that biological condition was significantly dependent (95% confidence level) on contaminants in vegetative habitats, but not on contaminants in sediments from the stream bottom. Biological condition was also significantly dependent on physical habitat quality; regression analysis on both contaminants and physical quality yielded the best regression model (r2 = 0.49). Similar biological impairment was observed at sites with severe contamination or physical impairment or with moderate chemical and physical impairment. These results have implications for the management of urban streams.

In a preliminary study, the uptake and the mobility of uranium (U) by black oak trees (Quercus velutina) were assessed by measuring the isotopic composition of tree rings in two mature oak trees in a heavy metal contaminated bog in Concord, MA. The bog is adjacent to a nuclear industrial facility that has been processing depleted uranium (DU) since 1959. Over the past 40 years, DU has been leaking from an onsite holding basin and cooling pond down gradient to the bog where the oaks are located. Because DU has no source outside the nuclear industry, contamination from the industrial facility is readily discernable from uptake of natural U by measuring isotopic compositions. Isotope ratio analysis confirms the occurrence of DU in bark, sapwood and heartwood tree rings dating back to 1937, pre-dating the introduction of DU at the site by at least 20 years. Isotope dilution analysis indicates high concentrations of U (>3 ppb) in sapwood that drop rapidly to relatively constant concentrations (0.3-0.4 ppb) in heartwood. These data indicate that once incorporated into tree cells, U is mobile, possibly by diffusion through the tree wood. Concentrations of U in sapwood are approximately equal to average U concentrations in groundwater onsite over the past 10 years, suggesting that oak trees can be used as present-day bioindicators of U-contaminated groundwater. We suggest that regional sampling of oak bark and sapwood is a reasonable, inexpensive alternative to drilling wells to monitor shallow groundwater U contamination.

Arsenic (As) mobility and transport in the environment are strongly influenced by arsenic's associations with solid phases in soil and sediment. We have tested a sequential extraction procedure intended to differentiate the following pools of solid phase arsenic: loosely and strongly adsorbed As; As coprecipitated with metal oxides or amorphous monosulfides; As coprecipitated with crystalline iron (oxyhydr)oxides; As oxides; As coprecipitated with pyrite; and As sulfides. Additions of As-bearing phases to wetland and riverbed sediment subsamples were quantitatively recovered by the following extractants of the sequential extraction procedure: As adsorbed on goethite, 1 M NaH2PO4; arsenic trioxide (As2O3), 10 M HF; arsenopyrite (FeAsS), 16 N HNO3; amorphous As sulfide, 1 N HCI, 50 mM Ti-citrate-EDTA, and 16 N HNO3; and orpiment (As2S3), hot concentrated HNO3/H2O2. Wet sediment subsamples from both highly contaminated wetland peat and less As-rich sandy riverbed sediment were used to test the extraction procedure for intra-method reproducibility. The proportional distribution of As among extractant pools was consistent for subsamples of the wetland and for subsamples of the riverbed sediments. In addition, intermethod variability between the sequential extraction procedure and a single-step hot concentrated HNO3/H2O2 acid digestion was investigated. The sum of the As recovered in the different extractant pools was not significantly different than results for the acid digestion.

Reconstructing the history of ambient levels of metals by using tree-ring chemistry is controversial. This controversy can be resolved in part through the use of selective microanalysis of individual wood cells. Using a combination of instrumental neutron activation analysis and secondary ion mass spectrometry, we have observed systematic inhomogeneity in the abundance of toxic metals (Cr, As, Cd, and Pb) within annual growth rings of Quercus rubra (red oak) and have characterized individual xylem members responsible for introducing micrometer-scale gradients in toxic metal abundances. These gradients are useful for placing constraints on both the magnitude and the mechanism of heavy metal translocation within growing wood. It should now be possible to test, on a metal-by-metal basis, the suitability of using tree-ring chemistries for deciphering long-term records of many environmental metals.