Long-term evolution of Fe oxyhydroxide mineralogy and potentially toxic element partitioning in mining-impacted sediments of the Lower Doce River fluvial-estuarine system.

IF 4.3 3区 环境科学与生态学 Q3 ENGINEERING, ENVIRONMENTAL
Danilo de Lima Camêlo, Gabriel da Silva Abreu Souza, David Lukas de Arruda, Sara Ramos Dos Santos, Poliana Borges de Oliveira, Maria Tereza Weitzel Dias Carneiro, Tiago Guimarães
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引用次数: 0

Abstract

The collapse of the Fundão dam in southeastern Brazil released large quantities of Fe-rich tailings into the Doce River basin, generating a long-term legacy of mining-derived sediments enriched in potentially toxic elements (PTEs). Although Fe oxyhydroxides are recognized as major geochemical hosts of contaminants, their long-term mineralogical evolution and relationships with PTE partitioning in tropical fluvial-estuarine systems remain poorly understood. This study investigated the distribution, crystallographic properties, and geochemical behavior of Fe oxyhydroxides in sediments collected from reservoir and estuarine environments of the lower Doce River between 2019 and 2024. Selective dissolution procedures, X-ray diffraction, diffuse reflectance spectroscopy, magnetic susceptibility measurements, and multivariate analyses were used to characterize Fe oxyhydroxide assemblages and their relationships with the investigated PTEs. Crystalline Fe oxyhydroxides predominated throughout the study area, although temporal variations in Fe partitioning were consistent with ongoing mineralogical reorganization across contrasting depositional environments. Higher Feo/Fed ratios at specific estuarine stations indicated relative enrichment of poorly crystalline Fe phases. Goethite remained the dominant Fe oxyhydroxide, whereas hematite exhibited greater spatial and temporal variability. Variations in crystal size, specific surface area, and Al substitution further suggest that Fe oxyhydroxide properties continue to evolve under present-day environmental conditions. Principal component analysis revealed strong associations between Fe oxyhydroxides and several PTEs, including As, Cr, Ni, Co, Pb, Zn, and Mo. The results indicate that Fe oxyhydroxides in mining-impacted sediments remain major geochemical hosts of the investigated PTEs more than a decade after the disaster, with their temporal variability closely associated with trace-element partitioning and potential redistribution. These findings highlight the importance of Fe mineralogy for understanding trace-element partitioning and potential redistribution and reinforce the value of mineralogical indicators and selective extraction procedures within long-term environmental monitoring frameworks.

下多斯河河河口水系采动沉积物中铁氧化铁矿物学的长期演化及潜在有毒元素分配
巴西东南部fund o大坝的倒塌向多塞河流域释放了大量富铁尾矿,形成了富含潜在有毒元素(pte)的采矿衍生沉积物的长期遗产。虽然铁氧氢氧化物被认为是污染物的主要地球化学宿主,但它们的长期矿物学演化及其与热带河流-河口系统PTE分配的关系仍然知之甚少。本文研究了2019 - 2024年在多斯河下游水库和河口环境中收集的沉积物中铁氧氢氧化物的分布、晶体学性质和地球化学行为。采用选择性溶解法、x射线衍射、漫反射光谱、磁化率测量和多变量分析来表征铁氧氧化铁组合及其与所研究pte的关系。尽管铁分配的时间变化与不同沉积环境中正在进行的矿物学重组相一致,但结晶铁氧化物在整个研究区域占主导地位。在特定的河口站,较高的Feo/Fed比值表明较差结晶的Fe相相对富集。氧化铁以针铁矿为主,赤铁矿表现出较大的时空变异性。晶体尺寸、比表面积和Al取代的变化进一步表明,在当今的环境条件下,铁的氢氧化物性质继续演变。主成分分析显示,铁氧化物与As、Cr、Ni、Co、Pb、Zn和Mo等几种pte之间存在较强的相关性。结果表明,灾后10多年,受采矿影响的沉积物中的铁氧化物仍然是所调查pte的主要地球化学宿主,其时间变化与微量元素分配和潜在再分配密切相关。这些发现强调了铁矿物学对理解微量元素分配和潜在再分配的重要性,并加强了矿物学指标和长期环境监测框架中选择性提取程序的价值。
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来源期刊
Environmental Geochemistry and Health
Environmental Geochemistry and Health 环境科学-工程:环境
CiteScore
8.00
自引率
4.80%
发文量
279
审稿时长
4.2 months
期刊介绍: Environmental Geochemistry and Health publishes original research papers and review papers across the broad field of environmental geochemistry. Environmental geochemistry and health establishes and explains links between the natural or disturbed chemical composition of the earth’s surface and the health of plants, animals and people. Beneficial elements regulate or promote enzymatic and hormonal activity whereas other elements may be toxic. Bedrock geochemistry controls the composition of soil and hence that of water and vegetation. Environmental issues, such as pollution, arising from the extraction and use of mineral resources, are discussed. The effects of contaminants introduced into the earth’s geochemical systems are examined. Geochemical surveys of soil, water and plants show how major and trace elements are distributed geographically. Associated epidemiological studies reveal the possibility of causal links between the natural or disturbed geochemical environment and disease. Experimental research illuminates the nature or consequences of natural or disturbed geochemical processes. The journal particularly welcomes novel research linking environmental geochemistry and health issues on such topics as: heavy metals (including mercury), persistent organic pollutants (POPs), and mixed chemicals emitted through human activities, such as uncontrolled recycling of electronic-waste; waste recycling; surface-atmospheric interaction processes (natural and anthropogenic emissions, vertical transport, deposition, and physical-chemical interaction) of gases and aerosols; phytoremediation/restoration of contaminated sites; food contamination and safety; environmental effects of medicines; effects and toxicity of mixed pollutants; speciation of heavy metals/metalloids; effects of mining; disturbed geochemistry from human behavior, natural or man-made hazards; particle and nanoparticle toxicology; risk and the vulnerability of populations, etc.
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