Arsenic contamination of shallow groundwater is among the biggest health threats in the developing world. Targeting uncontaminated deep aquifers is a popular mitigation option although its long-term impact remains unknown. Here we present the alarming results of a large-scale groundwater survey covering the entire Red River Delta and a unique probability model based on three-dimensional Quaternary geology. Our unprecedented dataset reveals that ∼7 million delta inhabitants use groundwater contaminated with toxic elements, including manganese, selenium, and barium. Depth-resolved probabilities and arsenic concentrations indicate drawdown of arsenic-enriched waters from Holocene aquifers to naturally uncontaminated Pleistocene aquifers as a result of >100 years of groundwater abstraction. Vertical arsenic migration induced by large-scale pumping from deep aquifers has been discussed to occur elsewhere, but has never been shown to occur at the scale seen here. The present situation in the Red River Delta is a warning for other As-affected regions where groundwater is extensively pumped from uncontaminated aquifers underlying high arsenic aquifers or zones.three-dimensional risk modeling | anthropogenic influence | drinking water resources | geogenic contamination | health threat
Groundwater drawn daily from shallow alluvial sands by millions of wells over large areas of South and Southeast Asia exposes an estimated population of over 100 million to toxic levels of arsenic (1). Holocene aquifers are the source of widespread arsenic poisoning across the region (2, 3). In contrast, Pleistocene sands deposited in this region more than ~12,000 years ago mostly do not host groundwater with high levels of arsenic. Pleistocene aquifers are increasingly used as a safe source of drinking water (4) and it is therefore important to understand under what conditions low levels of arsenic can be maintained. Here we reconstruct the initial phase of contamination of a Pleistocene aquifer near Hanoi, Vietnam. We demonstrate that changes in groundwater flow conditions and the redox state of the aquifer sands induced by groundwater pumping caused the lateral intrusion of arsenic contamination over 120 m from Holocene aquifer into a previously uncontaminated Pleistocene aquifer. We also find that arsenic adsorbs onto the aquifer sands and that there is a 16–20 fold retardation in the extent of the contamination relative to the reconstructed lateral movement of groundwater over the same period. Our findings suggest that arsenic contamination of Pleistocene aquifers in South and Southeast Asia as a consequence of increasing levels of groundwater pumping have been delayed by the retardation of arsenic transport.
Many aquifers that are highly contaminated by arsenic in South and Southeast Asia are in the floodplains of large river networks. Under natural conditions, these aquifers would discharge into nearby rivers; however, large‐scale groundwater pumping has reversed the flow in some areas so that rivers now recharge aquifers. At a field site near Hanoi Vietnam, we find river water recharging the aquifer becomes high in arsenic, reaching concentrations above 1000 µg/L, within the upper meter of recently (< ∼10 years) deposited riverbed sediments as it is drawn into a heavily pumped aquifer along the Red River. Groundwater arsenic concentrations in aquifers adjacent to the river are largely controlled by river geomorphology. High (>50 µg/L) aqueous arsenic concentrations are found in aquifer regions adjacent to zones where the river has recently deposited sediment and low arsenic concentrations are found in aquifer regions adjacent to erosional zones. High arsenic concentrations are even found adjacent to a depositional river reach in a Pleistocene aquifer, a type of aquifer sediment which generally hosts low arsenic water. Using geochemical and isotopic data, we estimate the in situ rate of arsenic release from riverbed sediments to be up to 1000 times the rates calculated on inland aquifer sediments in Vietnam. Geochemical data for riverbed porewater conditions indicate that the reduction of reactive, poorly crystalline iron oxides controls arsenic release. We suggest that aquifers in these regions may be susceptible to further arsenic contamination where riverine recharge drawn into aquifers by extensive groundwater pumping flows through recently deposited river sediments before entering the aquifer.
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