Department Water Resources and Drinking Water

Biogeochemical gas production resulting in free gas phase formation can severely affect groundwater and solute transport in aquifers. Such gas–water interactions are important in aquifers affected by geogenic As, which are commonly associated with biogeochemical CH₄ production. Additionally, the influence of aquitards on As concentrations in contaminated aquifers has recently been challenged. These observations prompted the analysis through a heterogeneous aquitard overlying a high CH₄-gas-producing zone of an As-contaminated aquifer. A sediment core taken through the aquitard was analyzed for noble gases to assess how the aquitard physically contributes to the underlying gas production. Results reveal that the aquitard pore space is unsaturated in two separate layers resulting in hanging pore water constrained by an air-like gas phase. This interlayering of unsaturated and saturated zones identifies the aquitard's stratigraphy as key in determining hydrostatic pressure - a main control of free gas formation (i.e., CH₄) in the underlying aquifer. The partly unsaturated conditions reduce the hydrostatic pressure by 30% compared with fully saturated conditions. To our knowledge, this is the first study applying noble gases to examine the influence of an aquitards physical state on gas production in an underlying aquifer. Further, such partly unsaturated sediment layers of low conductivity might provide preferential pathways for periodic water flow, fostering aquitard–aquifer solute transport. Groundwater samples additionally collected throughout the study site confirm more widespread degassing than previously reported. Up to 90% of the expected atmospheric noble gas concentrations is lost from groundwater immediately below the investigated sediment core.

Known locally as the water mountain, for millennia Japan’s iconic Mt Fuji has provided safe drinking water to millions of people via a vast network of groundwater and freshwater springs. Groundwater, which is recharged at high elevations, flows down Fuji’s flanks within three basaltic aquifers, ultimately forming countless pristine freshwater springs among Fuji’s foothills. Here we challenge the current conceptual model of Fuji being a simple system of laminar groundwater flow with little to no vertical exchange between its three aquifers. This model contrasts strongly with Fuji’s extreme tectonic instability due to its unique location on top of the only known continental trench–trench–trench triple junction, its complex geology and its unusual microbial spring water communities. On the basis of a unique combination of microbial environmental DNA, vanadium and helium tracers, we provide evidence for prevailing deep circulation and a previously unknown deep groundwater contribution to Fuji’s freshwater springs. The most substantial deep groundwater upwelling has been found along Japan’s most tectonically active region, the Fujikawa-kako Fault Zone. Our findings broaden the hydrogeological understanding of Fuji and demonstrate the vast potential of combining environmental DNA, on-site noble gas and trace element analyses for groundwater science.

In this study, the speciation and isotopic composition of Zn were traced across the sediments of a freshwater lake that experienced one hundred years of strong eutrophication, in order to assess the potential of sedimentary Zn isotopes to record such an environmental disturbance. The results indicate that the sedimentary Zn isotope signal varied with the change from pre-eutrophic to eutrophic conditions in the investigated lake. The average δ⁶⁶Zn_JMC value of the dominantly allochthonous lithogenic sediments deposited during the pre-eutrophic period was +0.27‰ ±0.05‰ (i.e. similar to the δ⁶⁶Zn_JMC value of +0.28‰ ±0.05‰ proposed for Bulk Silicate Earth), while enhanced autochthonous biochemical sedimentation during the eutrophic period resulted in significantly lower δ⁶⁶Zn_JMC values down to +0.04‰ ±0.06‰. Synchrotron-based X-ray absorption spectroscopy data revealed a concomitant change in Zn speciation from a dominant fraction of Zn in clay minerals during the pre-eutrophic period to a major fraction of Zn in ZnS during the eutrophic period. A linear regression relating the sedimentary Zn isotope signal to the fraction of Zn in ZnS indicated δ⁶⁶Zn_JMC values of +0.27‰ ±0.06‰ and 0.00‰ ±0.08‰ for Zn in clay minerals and in ZnS, respectively. The enrichment of light Zn in ZnS in the eutrophic sediments is tentatively attributed to enhanced biological uptake of light Zn in the water column, which resulted in an enhanced flux of organic-bound Zn towards the sediments and further transformation of organic Zn into ZnS upon biomass mineralization during early diagenesis. This hypothesis is in agreement with the fractionation towards lighter Zn reported for both biological uptake of Zn and ZnS precipitation. The results of this study emphasize the potential of sedimentary Zn isotopes to register past eutrophic periods in freshwater lakes, and thus to serve as a probe of paleo-environmental conditions and/or past land use at the catchment scale.