Molecular characteristics of dissolved organic matter regulate the binding and migration of tungsten in porous media.

IF 8.2 1区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Science of the Total Environment Pub Date : 2024-12-01 Epub Date: 2024-10-02 DOI:10.1016/j.scitotenv.2024.176670
Weijun Li, Jian Xie, Rui Huang, Wei Chen, Huihui Du
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Abstract

Tungsten (W) is an emerging contaminant that poses potential risks to both the environment and human health. While dissolved organic matter (DOM) can significantly influence the W's environmental behavior in natural aquifers, the mechanisms by which DOM's molecular structure and functional group diversity impact W binding and migration remain unclear. Using molecular weight-fractionated soil and sediment DOM (<1 kDa, 1-100 kDa, and 100 kDa-0.45 μm), this study systematically investigated the relationship between DOM molecular characteristics and tungstate (WO42-) binding properties using multiple spectroscopic methods, including FTIR, fluorescence spectroscopy and XPS. The migration behavior of WO42- in porous media was also investigated through quartz sand column experiments. Results revealed that approximately 75 % of W was controlled by DOM, with over 50 % binding to low molecular weight DOM (<1 kDa). Tungsten bound to medium-high molecular weight DOM (1-100 kDa, >100 kDa) showed a greater propensity for retention, with the >100 kDa fractions demonstrating stronger selective binding to W, exhibiting distribution coefficients (Kmd) of 6.11 L/g and 10.69 L/g, respectively. Further analysis indicated that W primarily binds with aromatic rings, phenolic hydroxyls, polysaccharides, and carboxyl groups in DOM, potentially affecting DOM structural stability and consequently influencing W migration characteristics. Free W migration in quartz sand was primarily controlled by Langmuir monolayer adsorption, leading to local enrichment (Da = 6.83, Rd = 86.98). When bound to DOM, W's migration ability significantly increased (Rd = 8-10), with adsorption shifting to a Freundlich multilayer model, primarily controlled by convective transport (Npe = 27-62> > 1.96), while adsorption effects weakened (Da ≈ 1). This study, for the first time, systematically reveals the regulatory mechanisms of DOM molecular characteristics on tungsten's environmental behavior. It offers crucial parameter support for constructing tungsten migration models and provides important guidance for tungsten pollution risk assessment and remediation strategies.

溶解有机物的分子特征调节钨在多孔介质中的结合和迁移。
钨(W)是一种新出现的污染物,对环境和人类健康都有潜在风险。虽然溶解有机物(DOM)能显著影响钨在天然含水层中的环境行为,但 DOM 的分子结构和官能团多样性对钨的结合和迁移的影响机制仍不清楚。本研究采用多种光谱方法(包括傅立叶变换红外光谱、荧光光谱和 XPS)研究了从土壤和沉积物中提取的 DOM(分为 42-)的结合特性。通过石英砂柱实验研究了 DOM 分子特性对 WO42- 在多孔介质中迁移的影响。结果显示,约 75% 的 W 受 DOM 控制,其中 50% 以上与低分子量 DOM(100 kDa)结合,显示出更大的保留倾向,而 >100 kDa 的馏分与 W 的选择性结合更强,其分布系数 (Kmd) 分别为 6.11 L/g 和 10.69 L/g。进一步分析表明,W 主要与 DOM 中的芳香环、酚羟基、多糖和羧基结合,可能会影响 DOM 结构的稳定性,从而影响 W 的迁移特性。W 在石英砂中的自由迁移主要受朗缪尔单层吸附控制,导致局部富集(Da = 6.83,Rd = 86.98)。当与 DOM 结合时,W 的迁移能力明显增强(Rd = 8-10),吸附转变为 Freundlich 多层模型,主要由对流传输控制(Npe = 27-62> > 1.96),而吸附效应减弱(Da ≈ 1)。这项研究首次系统地揭示了 DOM 分子特征对钨环境行为的调控机制。它为构建钨迁移模型提供了重要的参数支持,为钨污染风险评估和修复策略提供了重要指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Science of the Total Environment
Science of the Total Environment 环境科学-环境科学
CiteScore
17.60
自引率
10.20%
发文量
8726
审稿时长
2.4 months
期刊介绍: The Science of the Total Environment is an international journal dedicated to scientific research on the environment and its interaction with humanity. It covers a wide range of disciplines and seeks to publish innovative, hypothesis-driven, and impactful research that explores the entire environment, including the atmosphere, lithosphere, hydrosphere, biosphere, and anthroposphere. The journal's updated Aims & Scope emphasizes the importance of interdisciplinary environmental research with broad impact. Priority is given to studies that advance fundamental understanding and explore the interconnectedness of multiple environmental spheres. Field studies are preferred, while laboratory experiments must demonstrate significant methodological advancements or mechanistic insights with direct relevance to the environment.
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Sodium tungstate dihydrate (Na2WO4·2H2O)
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