长期淹没-浮出交替对沉积物-水系统中全氟烷基和多氟烷基物质（PFASs）命运的影响：来自溶解有机物的见解

IF 7.3 2区环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES

Environmental Pollution Pub Date : 2025-07-11 DOI:10.1016/j.envpol.2025.126822

Ye-bing Shi , Zu-lin Hua , Zi-wei Chen

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引用次数: 0

摘要

长期的浮潜交替在全球水循环中具有普遍的生态环境意义。然而，在这一过程中，溶解有机物（DOM）与全氟烷基和多氟烷基物质（PFASs）之间相互作用的认识有限。本研究通过长期浸没-浮出交替（ASE）与持续浸没（CS）的对比实验，探讨了污染沉积物中全氟烷基物质（PFASs）和多氟烷基物质（PFASs）的释放，并利用光谱技术和高分辨率质谱技术揭示了DOM在这一过程中的贡献。结果表明，长期的淹出交替极大地促进了污染沉积物中PFAS的释放和向水相的迁移。ASE组沉积物中∑PFAS浓度为437.8 μg/kg dw，比CS组的774.93 μg/kg dw降低了66.32%，比CS组降低了40.39%。ASE组孔隙水和上覆水中∑PFAS浓度（1592.51±18.11 μ L和458.06±32.52 μ L）显著高于CS组（1073.94±39.08 μ L和235.26±8.10 μ L），其中短链PFAS浓度最高。电喷雾电离傅里叶变换离子回旋共振质谱和DOM的光谱分析表明，长期的淹出交替使DOM的组成和特征发生了很大的变化。NOSC（-0.34）、DBE（8.43）、AImod>；0.5和O/C（0.4335）值越高，DOM极性越强，芳香性越强，稳定性越差。蛋白质和CHOS配方化合物的减少减少了共吸附，羧基和羟基丰度的增加加剧了PFASs和DOM之间的竞争吸附，这可能是长期淹出交替影响沉积物PFAS释放的潜在机制。这些发现为长期淹没-出露交替作用下DOM和PFASs的沉积地球化学循环提供了新的认识。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Impact of long-term submerge-emerge alternation on the fate of per- and polyfluoroalkyl substances (PFASs) in sediment-water systems: Insight from dissolved organic matter

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Impact of long-term submerge-emerge alternation on the fate of per- and polyfluoroalkyl substances (PFASs) in sediment-water systems: Insight from dissolved organic matter

Long-term submerge-emerge alternations have universal eco-environmental significance in the global aquatic cycle. However, the insight of interaction between dissolved organic matter (DOM) and per- and polyfluoroalkyl substances (PFASs) within this process is limited. In this study, through comparative experiments of long-term submerge-emerge alternation (ASE) versus continued submergence (CS), we explored the release of per- and polyfluoroalkyl substances (PFASs) from contaminated sediment and used spectral technologies and high-resolution mass spectrometry to reveal the DOM contribution in this process. Results indicated that long-term submerge-emerge alternation greatly enhanced PFAS release from contaminated sediments and their migration into aqueous phases. In the ASE group, the ∑PFAS concentration in sediment decreased to 437.8 μg/kg dw, a reduction of 66.32 %, compared with 774.93 μg/kg dw in the CS group, representing a decrease of 40.39 %. The ∑PFAS concentrations in porewater and overlying water were significantly higher in the ASE group (1592.51 ± 18.11 μg/L and 458.06 ± 32.52 μg/L) compared with those in the CS group (1073.94 ± 39.08 μg/L and 235.26 ± 8.10 μg/L), particularly for short-chain PFASs. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry and spectral analysis of DOM revealed that long-term submerge-emerge alternation substantially altered the DOM composition and characteristics. Specifically, the higher NOSC (−0.34), DBE (8.43), AI_mod>0.5, and O/C (0.4335) values indicated stronger polarity, increased aromaticity, and reduced stability of DOM. The decreased presence of protein and CHOS formula compounds reduced co-adsorption, and the increased abundance of carboxyl and hydroxyl groups intensified competitive adsorption between PFASs and DOM could be the potential mechanism by which long-term submerge-emerge alternation affected sediment PFAS release. These findings provide novel insights into the sedimentary geochemical cycling of DOM and PFASs under long-term submerge-emerge alternation.

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来源期刊

Environmental Pollution 环境科学-环境科学

CiteScore

16.00

自引率

6.70%

发文量

2082

审稿时长

2.9 months

期刊介绍： Environmental Pollution is an international peer-reviewed journal that publishes high-quality research papers and review articles covering all aspects of environmental pollution and its impacts on ecosystems and human health. Subject areas include, but are not limited to: • Sources and occurrences of pollutants that are clearly defined and measured in environmental compartments, food and food-related items, and human bodies; • Interlinks between contaminant exposure and biological, ecological, and human health effects, including those of climate change; • Contaminants of emerging concerns (including but not limited to antibiotic resistant microorganisms or genes, microplastics/nanoplastics, electronic wastes, light, and noise) and/or their biological, ecological, or human health effects; • Laboratory and field studies on the remediation/mitigation of environmental pollution via new techniques and with clear links to biological, ecological, or human health effects; • Modeling of pollution processes, patterns, or trends that is of clear environmental and/or human health interest; • New techniques that measure and examine environmental occurrences, transport, behavior, and effects of pollutants within the environment or the laboratory, provided that they can be clearly used to address problems within regional or global environmental compartments.