Spatiotemporal Variability of Groundwater Iodine in the Northern Arid Basins: Significance for Safe Water Supply.

The genesis of geogenic iodine (I)-contaminated groundwater poses a significant threat to long-term water exploitation. Safe and sustainable water supply, particularly in the northern arid basins, demands a quantitative prediction of the high variability of I distribution over hydrogeological timescales. Here, bioenergetics-informed reactive transport modeling was combined with high-resolution molecular characterization of fueling organic matter to decipher the time-controlled interactions between vertical flow and (bio)geochemical processes in I transport within the Datong aquifers. The declining reactivities of I-bearing organic matter and Fe oxides in the 15-40 m depth decreased the rate of I release, while a growing number of pore volumes flushed through the aquifers to leach out I - and organic I. This removal effect is compensated by the desorption of I - from Fe oxides and secondary FeS generated from the concurrent reduction of Fe oxides and SO 4 2- . Consequently, peak concentrations of groundwater I - may have appeared, depending upon the vertical recharge rate, at the first several pore volumes flushed through the aquifers. The current vertical distributions of the various I species likely represent a quasi-steady state between I mobilization and leaching. These new mechanistic insights into the dynamic hydrogeological-(bio)geochemical processes support secure groundwater use in the I-affected northern arid basins.