内蒙古岱海表层沉积物氟化物赋存特征及基于吸附解吸动力学影响因素分析
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内蒙古农业大学水利与土木建筑工程学院

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国家自然基金重点项目区域联合基金(U24A20633)、内蒙古自治区科技计划项目(2023YFHH0060)、国家自然科学基金(52260029)、内蒙古自治区教育厅科技英才项目(NJYT22040)、内蒙古农业大学青年教师科研能力提升基金(BR220102)和内蒙古自然科学基金(2022MS05053,2024QN05005)联合资助


Analysis of Fluoride Occurrence Characteristics and Influencing Factors in Surface Sediments of Daihai Lake: Coupling Verification Based on Orthogonal Experiments and Adsorption Models
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Water Conservancy and Civil Engineering College, Inner Mongolia Agricultural University

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Jointly funded by the National Natural Science Foundation Key Project Regional Joint Fund (U24A20633), Inner Mongolia Autonomous Region Science and Technology Plan Project (2023YFHH0060), National Natural Science Foundation (52260029), Inner Mongolia Autonomous Region Education Department Science and Technology Talent Project (NJYT22040), Inner Mongolia Agricultural University Young Teachers

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    摘要:

    内蒙古分布的众多湖泊受到环境变化影响出现氟化物浓度超标问题,对人体和湖泊产生致癌性健康风险和潜在生态环境风险。为了深入探讨湖泊沉积物中氟化物的赋存形态特征,揭示氟化物的吸附-解吸行为与影响因素之间的响应关系。以岱海为研究对象,采集表层沉积物样品,通过多级提取检测不同形态氟化物含量,应用ArcGIS软件进行氟化物时空差异性分析,进一步设计了4因素、3水平沉积物氟化物吸附-解吸正交模拟和吸附-解吸动力学模型模拟实验,揭示环境因子对寒旱区湖泊氟化物吸附和解吸行为的影响。结果表明:岱海沉积物中总氟含量均值为860.44±53.64 mg·kg-1,变化范围为600.03~1388.67 mg·kg-1。其中,水溶态、可交换态、铁锰结合态、有机束缚态氟化物含量变化范围分别为29.51~42.87 mg·kg-1,8.37~21.81 mg·kg-1,2.46~7.21 mg·kg-1,9.79~17.59 mg·kg-1之间。对沉积物氟化物吸附-解吸过程拟合分析得出,不同初始浓度条件下,准二级动力学模型拟合度更高,能够更好地表征该吸附体系的动力学过程;选用Langmuir、Freundlich两种热力学模型拟合分析氟化物吸附行为,证实吸附过程中单层吸附起关键作用,而非均相表面的多分子层吸附也是影响吸附行为的重要因素;进一步通过正交实验数据极差分析和方差分析,确定了各环境因素对吸附效果的影响程度和显著性。其中,温度是氟化物吸附-解吸的核心驱动因子(ANOVA显著性:温度>初始浓度>扰动强度>pH)。根据k值筛选出最优条件:初始浓度10 mg·L-1,温度20 ℃,pH=7,震荡频率200 r·min-1。本研究可为寒旱区湖泊沉积物氟释放污染防控提供重要的理论支撑。

    Abstract:

    The numerous lakes distributed in Inner Mongolia have experienced problems of excessive fluoride concentration due to environmental changes, posing carcinogenic health risks to humans and the lakes themselves, as well as potential ecological risks. To deeply explore the characteristics of fluoride forms in lake sediments and reveal the response relationship between fluoride adsorption-desorption behavior and influencing factors, Daihai Lake was selected as the research object. Surface sediment samples were collected, and the contents of different forms of fluoride were detected through multi-stage extraction. ArcGIS software was used to analyze the temporal and spatial differences of fluoride. Further, a 4-factor, 3-level orthogonal simulation experiment of fluoride adsorption-desorption in sediments and a simulation experiment of adsorption-desorption kinetics model were designed to reveal the influence of environmental factors on the adsorption and desorption behavior of fluoride in cold and arid lake sediments. The results showed that the average total fluoride content in the sediments of Daihai Lake was 860.44 ± 53.64 mg·kg-1, with a range of 600.03 to 1388.67 mg·kg-1. Among them, the content ranges of water-soluble, exchangeable, iron-manganese-bound, and organic-bound fluoride were 29.51 to 42.87 mg·kg-1, 8.37 to 21.81 mg·kg-1, 2.46 to 7.21 mg·kg-1, and 9.79 to 17.59 mg·kg-1, respectively. The fitting analysis of the fluoride adsorption-desorption process in sediments indicated that the pseudo-second-order kinetic model had a higher fitting degree under different initial concentrations and could better describe the kinetic process of this adsorption system. The Langmuir and Freundlich thermodynamic models were used to fit and analyze the fluoride adsorption behavior, confirming that monolayer adsorption played a key role in the adsorption process, while multilayer adsorption on heterogeneous surfaces was also an important factor affecting the adsorption behavior. Through the range analysis and variance analysis of orthogonal experimental data, the influence degree and significance of each environmental factor on the adsorption effect were determined. Among them, temperature was the core driving factor for fluoride adsorption-desorption (ANOVA significance: temperature > initial concentration > disturbance intensity > pH). The optimal conditions were screened out based on k values: initial concentration of 10 mg·L-1, temperature of 20 ℃, pH of 7, and shaking frequency of 200 r·min-1. This study can provide important theoretical support for the prevention and control of fluoride release pollution from lake sediments in cold and arid regions.

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  • 收稿日期:2025-07-10
  • 最后修改日期:2026-04-06
  • 录用日期:2025-09-04
  • 在线发布日期: 2025-11-04
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