Abstract

Highlights

  • Sediment fluoride (206.2 mg/kg to 780.9 mg/kg) exceeds the global average.
  • Fluoride in carbonate minerals decreases initially and then increases during stepwise dissolution.
  • Amorphous dolomite dissolves first, releasing loosely bound fluoride, followed by calcite and fully crystallized dolomite.
  • Silt loam releases most fluoride due to higher amorphous carbonate content, while sandy loam releases least.
  • The dissolution of carbonates regulates fluoride enrichment in groundwater.

A critical investigation in environmental science, examining the fluoride geochemistry of sediments from uniquely characterized fluoride-rich location. The investigation of sediment samples collected from Yuncheng Basin. This purposeful decision is based on the notion that the existence of water flow influences fluoride distribution and geochemical behavior in sediments. We want to understand fundamental patterns and processes that drive fluoride dynamics in these ecosystems by focusing our research on sediments.

Our findings reveal that the total fluoride content in sediments ranges from 624.6 to 1072.0 mg/kg, with higher concentrations observed in the middle sediment layers. The particle size analysis indicates a negative correlation between fluoride content and median particle size (d50), with finer particles showing higher fluoride adsorption. Sequential extraction procedures identified the dominant forms of fluoride in sediments, including water-soluble, ion-exchanged, carbonate-bound, Fe-Al-bound, and organically bound fluoride, with carbonate-bound fluoride being a significant contributor.

The study also highlights the influence of carbonate minerals and evaporated salts on fluoride mobilization and accumulation. Static leaching experiments demonstrate that fluoride release is significantly affected by the dissolution of carbonate minerals, driven by both water dissolution and acidic conditions. This research underscores the complex interplay between sediment lithology, mineral composition, and fluoride dynamics, providing valuable insights into the environmental processes governing fluoride contamination in groundwater.

Introduction

Fluoride contamination in groundwater is a significant environmental issue globally, with serious implications for human health and agriculture (Ali et al., 2016). In the Yuncheng Basin of Shanxi Province, China, fluoride contamination has been a pressing concern due to the region’s high fluoride levels in both groundwater and sediments (Hao et al., 2023; Li et al., 2015). Understanding the mechanisms of fluoride mobilization and its association with sediment characteristics is crucial for developing effective mitigation strategies.

Fluoride, a naturally occurring element, can become problematic when it accumulates in high concentrations (Edmunds and Smedley, 2012; Jha et al., 2011). Its mobilization in sediments and groundwater is influenced by various geochemical processes. Recent studies have highlighted the role of sediment composition, mineralogy, and particle size in fluoride distribution and mobility (Gao et al., 2024). For instance, Wang et al., 2023a, Wang et al., 2023b demonstrated that fine sediment particles have a higher fluoride adsorption capacity due to their larger surface area and higher reactivity (Wang et al., 2023a). Similarly it is investigated the role of carbonate minerals in fluoride retention and release, noting that carbonate-bound fluoride can significantly impact groundwater quality (Du et al., 2022).

The Yuncheng Basin, known for its high fluoride concentrations, offers a unique opportunity to study fluoride behavior in sedimentary environments. Previous research has identified elevated fluoride levels in groundwater, with concentrations often exceeding recommended limits for drinking water (Chen et al., 2021). This study aims to further investigate the fluoride geochemistry of sediments in the basin, focusing on the forms of fluoride present, their association with sediment properties, and the influence of carbonate minerals.

Recent advances in analytical techniques have enabled more precise assessments of fluoride in sediments. Methods such as sequential extraction procedures and advanced spectroscopic techniques have improved our understanding of fluoride speciation and distribution. For instance, sequential extraction has been applied to identify various fluoride forms, including carbonate-bound and Fe-Al-bound fluoride, providing insights into their environmental behavior (Gao et al., 2024).

While previous studies by Zhang et al. (2022) and Wang et al., 2023a, Wang et al., 2023b from our laboratory have examined the hydrogeochemical mechanisms and microbial contributions to fluoride mobilization in groundwater of the Yuncheng Basin, these works did not explore the relationships between sediment grain size and specific fluoride fractions. This is the first comprehensive study to quantitatively assess the correlation between fluoride speciation in sediments and grain size distribution in the Yuncheng Basin. This novel approach helps to understand better the geochemical behavior of fluoride under varying sedimentological conditions.

This study builds upon existing knowledge by analyzing sediment samples from a borehole in Shandongzhuang Village, Qijizhen, within the Yuncheng Basin. We employ a combination of alkali fusion-ion selective electrode methods, particle size analysis, and X-ray fluorescence spectroscopy to characterize sediment fluoride content and its associations with sediment composition. By examining the correlation between fluoride content and particle size, as well as the role of carbonate minerals in fluoride mobilization, this research aims to contribute to a deeper understanding of fluoride dynamics in contaminated sedimentary environments (Fig. 1).

Section snippets

Collection of sediments

During the research period, a borehole was drilled in Qijizhen near to Yuncheng Basin in Shanxi Province. Representative sediment samples at different depths were collected from the area. Specifically, the borehole was drilled in Shandongzhuang Village, Qijizhen (with a drilling depth of 55 m), and a total of 10 sediment samples were collected. After collection, the surface layer was immediately removed, and the samples were wrapped in polyethylene cling film, sealed in polyethylene bottles,

Sediment lithology and fluoride occurrence

Sediment samples were collected from a borehole at varying depths ranging from 0 to 55 m. The selection of sample depths was based on lithological changes, ensuring representative coverage of different sediment layers. The specific depths of the collected samples are listed in Table 2. According to the particle size of sediment, sediment particles can be divided into three different particle sizes: sand (50 um), silt (2–50 um), and clay (< 2 um) (Blott and Pye, 2012). According to the grain

Environmental implication

This study offers significant insights into the environmental geochemical behavior of fluoride in the sediments of the Yuncheng Basin, particularly in relation to fluoride fractionation, sediment lithology, and carbonate mineral interactions. By examining various forms of fluoride through sequential extraction, the research provides a comprehensive understanding of how different fluoride fractions (exchangeable, carbonate-bound, and residual) contribute to overall fluoride mobilization in

Conclusions

  • (1) The sediments of Yuncheng Basin have a high total fluoride content in sediments, which is higher than the average fluoride content of sediment samples in China. The soil is alkaline, and sediment conductivity shows a decreasing trend with depth. Among them, the sediment conductivity in the area is high (231.54 uS/cm).
  • (2) The total fluoride content in sediment samples from Qijizhen is negatively correlated with particle size. From the relationship between total fluoride in sediments and chemical

CRediT authorship contribution statement

Aqsa Naseem: Methodology, Writing – original draft, Data curation, Formal analysis, Visualization, Conceptualization. Wenting Luo: Investigation, Formal analysis. Chengcheng Li: Writing – review & editing. Xing Zhang: Methodology, Formal analysis. Xubo Gao: Conceptualization, Writing – review & editing, Data curation, Investigation, Methodology.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgment

This research was financially supported by the National Natural Science Foundation of China (No. 42172288, and 42272287), National Key Technologies Research and Development Program Project “Prevention and Control of Groundwater Pollution and Safe Utilization of Abandoned Coal Mines in Karst Areas in Northern China- Multi-Field Coupling and the Key Processes and Accurate Simulation of Groundwater Quality Evolution” (No. 2023YFC3710002) and Guangxi Key Science and Technology Innovation Base on

References (60)

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