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In recent decades, water quality problems that impact human health, especially groundwater pollution, have been intensely studied, and this has contributed to new ideas and policies around the world such as Low Impact Development (LID) and Superfund legislation. The fundamental to many of these problems is pollutant occurrence and migration in saturated porous media, especially in groundwater. Such environments often contain contrasting zones of high and low permeability with significant differences in hydraulic conductivity (~10−4 and 10−8 m/s, respectively). High-permeability zones (HPZs) represent the primary pathways for pollutant transport in groundwater, while low-permeability zones (LPZs) are often diffusion dominated and serve as both sinks and sources (i.e., via back-diffusion) of pollutants over many decades. In this review, concepts and mechanisms of solute source depletion, contaminant accumulation, and back-diffusion in high- and low-permeability systems are presented, and new insights gained from both experimental and numerical studies are analyzed and summarized. We find that effluent monitoring and novel image analysis techniques have been adroitly used to investigate temporal and spatial evolutions of contaminant concentration; simultaneously, mathematical models are constantly upscaled to verify, optimize and extend the experimental data. However, the spatial concentration data during back-diffusion lacks diversity due to the limitations of pollutant species in studies, the microscopic mechanisms controlling pollutant transformation are poorly understood, and the impacts of these reactions on contaminant back-diffusion are rarely considered. Hence, most simulation models have not been adequately validated and are not capable of accurately predicting pollutant fate and cleanup in realistic heterogeneous aquifers. Based on these, some hypotheses and perspectives are mentioned to promote the investigation of contaminant migration in high- and low-permeability systems in groundwater.

Pollutant accumulation in the low-permeability zones (LPZs) in groundwater systems is regarded as a secondary source, and its consequent back-diffusion can extend the timeframe of pump-and-treat remediation. However, the bioavailability and mobility of heavy metals and the medium characteristics can be changed during the process. This study investigated the accumulation and back-diffusion law of toxic metals and the effects of ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) on them by implementing a series of tank experiments. In these experiments, a cadmium solution was injected first, and deionized water or EDTA-2Na constantly washed the system consisting of different medium layers. The experimental results showed that the cadmium breakthrough curves had some concentration gradient reverse points where the curves fluctuated with elution by deionized water, which did not exist when EDTA-2Na was the eluent. In these scenarios, the mass of accumulated cadmium in the media before elution was large, with a value of 931 mg (153 mg/kg), when the low-permeability medium was clay. However, when EDTA-2Na was injected together with cadmium, the value dropped to 319 mg (52.3 mg/kg), greatly reducing the cadmium accumulation. Additionally, the use of EDTA-2Na as an eluent resulted in the appearance of a secondary peak in the breakthrough curve, showing that EDTA-2Na accelerated and centralized the back-diffusion. Notably, the reduced cadmium accumulation in LPZs with the elution by EDTA-2Na was partly due to a reduced adsorption capacity of the clay minerals. The above results can advance the technology related to pump-and-treat remediation.