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

基本信息

批准号：
10707895
负责人：
Alex Halliday
金额：
$ 18.89万
依托单位：
COLUMBIA UNIVERSITY HEALTH SCIENCES
依托单位国家：
美国
项目类别：
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/10707895
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 Impact 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 Pattern Play Population Precipitation Privatization Process Reaction Research Reservations Resolution Risk Risk Reduction 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 diagnostic tool drinking drinking water exposed human population geochemistry ground water human data mineralization noninvasive diagnosis novel novel marker oxidation programs remediation tool tribal community tribal lands uptake urinary

项目摘要

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总结强心脏研究 (SHS) 中调查的美洲原住民社区显示砷 (As) 含量明显较高，尿液中铀 (U) 和硒 (Se) 的浓度相对于美国人口的平均水平。接触危险金属混合物来自饮用经常被以上金属污染的地下水美国的部落土地通常与矿藏、铀矿和金属（金属）一致。在北部平原含水层中，饮用水中铀和砷的浓度升高反映了这一情况。含水层中自然发生的富集，以及部落社区项目 2 附近的采矿遗留物。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 的成分，因为这些元素对含水层中的氧化还原变化敏感，可以推断来源和控制 U 和 Se 的氧化还原化学过程控制其水溶液。地下水中的浓度；氧化物质具有流动性且有毒，而还原物质则具有流动性和毒性。溶解的 U 和 Se 的浓度受到多种过程的影响（例如稀释、吸附、分散度），并且是地下水中氧化还原诱导的命运和循环的不良指标。地下水中溶解的 U 和 Se 及其浓度对于研究氧化还原诱导的 (im)动员、追踪吸收和人体暴露我们将使用 U 和 Se 同位素比率来表征。地下水中的氧化还原反应，获取有关反应进程的独特机械信息。数据将帮助我们定义本地和更远端的来源，以及金属的运输和循环过程此外，我们将开发同位素示踪剂。受环境暴露影响的人体中 U 和 Se 循环的具体目标是： (1) 确定。地下水样品中 U 和 Se 的同位素比率或“同位素”的空间分布模式。项目 1 的高分辨率数据和模型，用于 U、As 和 Se 热点内部和周围的目标井我们还将确定这些热点周围的局部污染源和远端污染源。 (2) 确定地下水中自然发生的还原性 U 和 Se 去除水平并确定我们将根据 U 和 Se 同位素比率的时间演变确定潜在 As 释放的条件。描述 U 和 Se 的氧化还原转化以及多个地下水源（如果有）的潜在混合。 (3) 使用同位素示踪剂确定人体暴露于环境污染的程度。追踪饮用水中 U 和 Se 金属暴露的新型非侵入性方法为此，我们将测量 U。尿液中的 Se 同位素比率，通过将主要暴露源和受影响人群联系起来来限制主要暴露源和受影响人群水等景观和项目 3 的观测数据。我们的结果将有助于评估暴露于有害金属混合物、受污染含水层的监测和管理以及将暴露与使用非侵入性诊断工具检测环境来源。