Origin and Enrichment Mechanisms of Salinity and Fluoride in Sedimentary Aquifers of Datong Basin, Northern China

The exposure of inhabitants to high fluoride and saline groundwater is the main health issue in Datong Basin, Northern China. This study aims to elucidate the spatial distribution and the mechanisms of high fluoride and salinity occurrence in the shallow sedimentary aquifers of the Datong Basin. Groundwater salinity and fluoride content, and their association with measured hydrochemical parameters, were conducted using multivariate statistical analyses. The analytical results revealed that the concentrations of fluoride and total dissolved solids (TDS) show dramatic variations within the study area. Around 41.4% of groundwater samples contained high-level fluoride concentration (F(−) > 1.5 mg/L), whereas 32.8% contained elevated-level TDS (TDS > 1000 mg/L). Both fluoride and TDS concentrations had elevated trends towards the central part of the basin. Shallow groundwater was seriously affected by evaporation and evapotranspiration, which can be the critical factors responsible for rather high TDS and F(−) concentrations in shallow aquifers. Water–rock reactions including silicate hydrolysis, dissolution–precipitation of carbonates and evaporates, adsorption, and ion exchange processes, as well as evapotranspiration, are the main governing factors for salinity and fluoride enrichment in groundwater. Solubility control of F-bearing and carbonate minerals is the dominant mechanism affecting F(−) levels. Prevailing conditions of alkaline pH, moderate TDS and Na(+), high HCO(3)(−), and lower Ca(2+) content facilitate the enrichment of fluoride in the study area. Excessive evapotranspiration can be also the most influencing factor responsible for high fluoride and TDS content, due to the extended residence time of groundwater and the arid climate of the central part of the Datong Basin.