Abstract: Seawater intrusion (SWI) has led to salinization of fresh groundwater reserves in coastal areas worldwide and has forced the closure of water supply wells. There is a paucity of well-documented studies that report on the reversal of SWI after the closure of a well field. This study presents data from the coastal carbonate aquifer in northeast China, where large-scale extraction has ceased since 2001 after salinization of the main well field. The physical flow and concomitant hydrogeochemical processes were investigated by analyzing water level and geochemical data, including major ion chemistry and stable water isotope data. Seasonal water table and salinity fluctuations, as well as changes of δ2H–δ18O values of groundwater between the wet and dry season, suggest local meteoric recharge with a pronounced seasonal regime. Historical monitoring testifies of the reversibility of SWI in the carbonate aquifer, as evidenced by a decrease of the Cl− concentrations in groundwater following restrictions on groundwater abstraction. This is attributed to the rapid flushing in this system where flow occurs preferentially along karst conduits, fractures and fault zones. The partially positive correlation between δ18O values and TDS concentrations of groundwater, as well as high NO3− concentrations (\textgreater39mg/L), suggest that irrigation return flow is a significant recharge component. Therefore, the present-day elevated salinities are more likely due to agricultural activities rather than SWI. Nevertheless, seawater mixing with fresh groundwater cannot be ruled out in particular where formerly intruded seawater may still reside in immobile zones of the carbonate aquifer. The massive expansion of fish farming in seawater ponds in the coastal zone poses a new risk of salinization. Cation exchange, carbonate dissolution, and fertilizer application are the dominant processes further modifying the groundwater composition, which is investigated quantitatively using hydrogeochemical models.

Abstract: Understanding the interference of natural processes and anthropogenic activities in geochemical evolution of groundwater is vital for groundwater sustainable management in water-stressed regions. This study is devoted to the identification of the main factors controlling the evolution of groundwater chemistry by the combined use of hydrogeochemical indicators along with isotope tracers in the Heilongdong Spring Basin, North China. Thirty-nine groundwater samples and twelve surface water samples were collected, and major ions and stable isotopes were measured during the two campaigns (December 2017 and August 2018). The isotope approach indicates that the groundwater is recharged by precipitation infiltration after evaporation, and interacts with surface water along preferential flow paths in fault zones and karst conduits. Currently, the main chemical facies of groundwater evolve from Ca-HCO3 and Ca-Mg-HCO3 types with low TDS, through Ca-Mg-HCO3-SO4 and Ca-HCO3-SO4 types with moderate TDS, to Ca-SO4, Ca-SO4-Cl and CaCl types with high TDS. Apart from natural processes (involving dissolution/precipitation of minerals, cation exchange, and evaporation) regulating the groundwater quality, the stagnant zones also play a crucial role in the formation of severe localized nitrate contamination. The deterioration in groundwater quality can be attributed to anthropogenic factors (including the change in groundwater exploitation, the leaching of solid waste, and the overuse of agricultural fertilizers). The high loads of agricultural fertilizers in irrigation return flows are likely to be the main contributor of the dissolved nitrate in groundwater. The findings of this work not only have important implications for groundwater sustainable utilization, but also could serve as a template for other rapidly industrialized and water-stressed regions.