Isotopic Tracing of Sources and Cycling of Hazardous Metal Mixtures

危险金属混合物的同位素追踪和循环

• 批准号: 10354270
• 负责人: Anirban Basu
• 金额: $ 20.83万
• 依托单位: COLUMBIA UNIVERSITY HEALTH SCIENCES
• 依托单位国家: 美国
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-09-21 至 2027-06-30
• 项目状态: 未结题
• 来源: https://reporter.nih.gov/project-details/10354270
• 关键词: Adsorption; Affect; Area; Arsenic; Biological Markers; Cardiometabolic Disease; Characteristics; Chemicals; Chemistry; Cheyenne; Communities; Community Surveys; Data; Deposition; Development; Distal; Elements; Environment; Environmental Exposure; Environmental Pollution; Epidemic; Evolution; Excision; Exposure to; Fractionation; Geographic Distribution; Heart; Human; Human body; Immobilization; Intervention; Ions; Isotopes; Light; Link; Maps; Measurement; Measures; Metal exposure; Metals; Methods; Minerals; Mining; Modeling; Monitor; Mus; Native Americans; North Dakota; Organ; Oxidation-Reduction; Oxides; Pattern; Play; Population; Precipitation; Privatization; Process; Reaction; Research; Reservations; Resolution; Risk; Rivers; Role; Rural Community; Safety; Sampling; Selenium; Sioux Indians; Site; Solid; Source; South Dakota; Spatial Distribution; Superfund; Testing; Time trend; Tissue Sample; Tissues; Trace Elements; Tracer; Tribes; Universities; Uranium; Urine; Water; aqueous; base; diagnostic tool; drinking; drinking water; exposed human population; geochemistry; ground water; human data; mineralization; noninvasive diagnosis; northern plains; novel; novel marker; oxidation; programs; remediation; tool; tribal community; tribal lands; uptake; urinary

Project 2 Summary Native American communities surveyed in the Strong Heart Study (SHS) show markedly higher arsenic (As), uranium (U) and selenium (Se) concentrations in urine relative to the average US population. Much of the exposure to hazardous metal mixtures comes from drinking groundwater contaminated with metals often above safety standards. Tribal lands in the US often coincide with mineral deposits, U mining, and metal(loid) contamination in aquifers. In the Northern Plains, elevated concentrations of U and As in drinking water reflect naturally occurring enrichment in aquifers, as well as the legacy of mining near tribal communities. Project 2 of the Columbia University Northern Plains Superfund Research Program (CUNP-SRP) will use isotopic compositions of U and Se, as these elements are sensitive to redox changes in the aquifer, to infer sources and processes controlling contaminant exposures. Redox chemistry of U and Se controls their aqueous concentrations in groundwater; the oxidized species are mobile and toxic whereas the reduced species are insoluble. Concentrations of dissolved U and Se are affected by multiple processes (e.g., dilution, adsorption, dispersion) and are poor indicators of redox-induced fate and cycling in groundwater. Thus, isotope ratios of dissolved U and Se in groundwater, in tandem with concentrations, are invaluable for studying redox-induced (im)mobilization, and tracing uptake and human exposure. We will use U and Se isotope ratios to characterize redox reactions in groundwater, acquiring unique mechanistic information about the reaction progress. These data will help us define local and more distal sources, and the transport and cycling processes of metals in groundwater within the SHS communities in North/South Dakota. Furthermore, we will develop isotopic tracers of U and Se cycling in humans impacted by environmental exposures. The specific aims are to: (1) Determine spatial distribution pattern of isotope ratios or “isoscapes” of U and Se in groundwater samples. This will use high-resolution data and models from Project 1 to target wells within and around U, As and Se hotspots for isotopic characterization. We will also identify local versus distal sources of contamination around these hotspots. (2) Determine the levels of naturally occurring reductive U and Se removal from groundwater and identify conditions for potential As release based on the temporal evolution of U and Se isotope ratios. We will characterize the redox transformation of U and Se and potential mixing of multiple groundwater sources (if any). (3) Determine human exposure from the environmental contamination using isotopic tracers. We will develop a novel non-invasive method to track metal exposure from U and Se in drinking water. For this, we will measure U and Se isotope ratios in urine to constrain primary exposure sources and affected populations by linking those to water isoscapes and the observational data from Project 3. Our results will help evaluate risk of exposure to hazardous metal mixtures, monitoring and management of contaminated aquifers, and linking exposures to environmental sources using a non-invasive diagnostic tool.

项目2摘要 在强大心脏研究（SHS）中调查的美国原住民社区表明，砷明显更高（AS）， 相对于美国平均人群，尿液中的铀（U）和硒（SE）浓度。大部分 暴露于危险金属混合物中来自经常被上面的金属污染的饮用地下水 安全标准。美国的部落土地经常与矿藏，U开采和金属（LIE）一致 含水层中的污染。在北部平原，U浓度升高，饮用水中的浓度升高 自然发生在含水层中，以及在部落社区附近采矿的遗产。项目2 哥伦比亚大学北部平原超级基金研究计划（CUNP-SRP）将使用同位素 U和SE的组成，因为这些元素对含水层中的氧化还原变化敏感，以推断来源和 控制污染物暴露的过程。 U和SE的氧化还原化学控制其水性 地下水的浓度；氧化的物种是流动的，有毒的，而还原物种是 无法解决。溶解的U和SE的浓度受多种过程的影响（例如，稀释，吸附， 分散），并且是氧化还原引起的命运和地下水骑自行车的差。那是同位素比 溶解的U和SE在地下水中以浓度串联，对于研究氧化还原诱导的 （IM）动员，追踪吸收和人类暴露。我们将使用U和SE同位素比来表征 地下水中的氧化还原反应，获得了有关反应进展的独特机械信息。这些 数据将帮助我们定义本地和更多的刻度源，以及金属的运输和骑​​行过程 北达科他州SHS社区内的地下水。此外，我们将开发同位素示踪剂 在人类中的U和SE骑自行车受环境暴露影响。具体目的是：（1）确定 地下水样品中U和SE的同位素比的空间分布模式。这将使用 从项目1到U内部和周围的井的高分辨率数据和模型，AS和SE热点 同位素表征。我们还将确定这些热点周围污染物的局部污染物和远端来源。 （2）确定自然发生的u和SE从地下水中删除的水平，并确定 基于U和SE同位素比的暂时进化，作为释放的潜力条件。我们将 表征U和SE的氧化还原转化以及多个地下水源的潜在混合（如果有）。 （3）使用同位素示踪剂确定人类从环境污染中暴露。我们将发展一个 新颖的非侵入性方法，可以跟踪饮用水中U和SE的金属暴露。为此，我们将衡量 尿液中的SE同位素比通过联系这些来限制主要的暴露源和影响人群 与项目3的观察数据以及我们的结果有关，我们的结果将有助于评估暴露的风险 有害的金属混合物，受污染的含水层的监测和管理，并将暴露与 使用非侵入性诊断工具的环境来源。