Abstract:Managed aquifer recharge (MAR) systems are an efficient barrier for many contaminants. The biotransformation of trace organic chemicals (TOrCs) strongly depends on the redox conditions as well as on the dissolved organic carbon availability. Oxic and oligotrophic conditions are favored for enhanced TOrCs removal which is obtained by combining two filtration systems with an intermediate aeration step. In this study, four parallel laboratory-scale soil column experiments using different intermittent aeration techniques were selected to further optimize TOrCs transformation during MAR: no aeration, aeration with air, pure oxygen and ozone. Rapid oxygen consumption, nitrate reduction and dissolution of manganese confirmed anoxic conditions within the first filtration step, mimicking traditional bank filtration. Aeration with air led to suboxic conditions, whereas oxidation by pure oxygen and ozone led to fully oxic conditions throughout the second system. The sequential system resulted in an equal or better transformation of most TOrCs compared to the single step bank filtration system. Despite the fast oxygen consumption, acesulfame, iopromide, iomeprol and valsartan were degraded within the first infiltration step. The compounds benzotriazole, diclofenac, 4-Formylaminoantipyrine, gabapentin, metoprolol, valsartan acid and venlafaxine revealed a significantly enhanced removal in the systems with intermittent oxidation compared to the conventional treatment without aeration. Further improvement of benzotriazole and gabapentin removal by using pure oxygen confirmed potential oxygen limitation in the second column after aeration with air. Ozonation resulted in an enhanced removal of persistent compounds (i.e., carbamazepine, candesartan, olmesartan) and further increased the attenuation of gabapentin, methylbenzotriazole, benzotriazole, and venlafaxine. Diatrizoic acid revealed little degradation in an ozone-MAR hybrid system.

Bank filtration (BF) and soil aquifer treatment (SAT) are efficient natural technologies in potable water reuse systems. The removal of many organic micro-pollutants (OMPs) depends on redox-conditions in the subsoil, especially on the availability of molecular oxygen. Due to microbial transformation of particulate and dissolved organic constituents, oxygen can be consumed within short flow distances and induce anoxic and anaerobic conditions. The effect of accumulated particulate organic carbon (POC) on the fate of OMPs in BF and SAT systems is not fully understood. Long-term column experiments with natural sediment cores from the bank of Lake Tegel and from a SAT basin were conducted to investigate the impact of accumulated POC on dissolved organic carbon (DOC) release, on oxygen consumption, on mobilization of iron and manganese, and on the elimination of the organic indicator OMPs. The cores were fed with aerated tap water spiked with OMPs to exclude external POC inputs. Complete oxygen consumption within the first infiltration decimeter in lake sediments caused mobilization of iron, manganese, and DOC. Redox-sensitive OMPs like diclofenac, sulfamethoxazole, formylaminoantipyrine, and gabapentin were eliminated by more than 50% in all sediment cores, but slightly higher residual concentrations were measured in effluents from lake sediments, indicating a negative impact of a high oxygen consumption on OMP removal.

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Autochthonous carbon fixation by algae and subsequent deposition of particulate organic matter can have significant effects on redox conditions and elimination of trace organic chemicals (TOrCs) in managed aquifer recharge (MAR). This study investigated the impacts of different algae loadings (0–160 g/m2) and infiltration rates (0.06–0.37 m/d) on overall oxygen consumption and elimination of selected TOrCs (diclofenac, formylaminoantipyrine, gabapentin, and sulfamethoxazole) in adapted laboratory sand columns. An infiltration rate of 0.37 m/d in conjunction with an algae load of 80 g/m2 (dry weight) sustained oxic conditions in the sand bed and did not affect the degradation of TOrCs. Thus, the availability of easily degradable organic carbon from algae did not influence the removal of TOrCs at an influent concentration of 1 µg/L. In contrast, a lower infiltration rate of 0.20 m/d in combination with a higher algae loading of 160 g/m2 caused anoxic conditions for 30 days and significantly impeded the degradation of formylaminoantipyrine, gabapentin, sulfamethoxazole, and diclofenac. Especially the elimination of gabapentin did not fully recover within 130 days after pulsed algae deposition. Hence, measures like micro-sieving or nutrient control are required at bank filtration or soil aquifer treatment sites with low infiltration rates.

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High nitrate concentrations in wastewater treatment plant effluents and aquifers can challenge sequential biofiltration systems in preventing nitrite and gas formation in the sand bed, as well as to achieve the regulated limit value for nitrate in potable water reuse applications. This study investigates the introduction of electron donors in the form of organic fixed bed materials as an in-situ anoxic zone into sequential biofiltration systems. Laboratory batch and column tests with straw, soft wood, peat, polylactic acid (PLA), and polycaprolacton (PCL) revealed incomplete denitrification with a hydraulic retention time below 10 h, high organic carbon leaching, especially during the first three months, and gas accumulation within the filter bed. Therefore, ex-situ denitrification prior to oxic biofilters or in a defined side-stream treatment is recommended. No enhanced transformation of trace organic chemicals was observed under nitrate reducing conditions. Peat revealed a sorption potential for 5-methyl-benzotriazole, carbamazepine, benzotriazole, and metoprolol.