RESUMEN
For a novel approach of resource-efficient water reuse, a municipal wastewater treatment plant was extended at pilot scale for advanced wastewater treatment, i.e., ozonation and biological activated carbon filtration, and a hydroponic system for reclaimed water driven lettuce cultivation. The treatment specific wastewater lines with the corresponding lettuce plants, differentiated into roots and shoots, were monitored for priority wastewater micropollutants, i.e., acesulfame (sweetener), caffeine (stimulant), carbamazepine, diclofenac, ibuprofen, sulfamethoxazole with acetyl-sulfamethoxazole (human pharmaceuticals), 1H-benzotriazole, and 4/5-methylbenzotriazole (industrial chemicals). As clearly demonstrated, conventional tertiary treatment could not efficiently clean up wastewater. Removal efficiencies ranged from 3% for carbamazepine to 100% for ibuprofen. The resulting pollution of the hydroponic water lines led to the accumulation of acesulfame, carbamazepine, and diclofenac in lettuce root systems at 32.0, 69.5, and 135 µg kg-1 and in the uptake of acesulfame and carbamazepine into lettuce shoots at 23.4 and 120 µg kg-1 dry weight, respectively. In contrast, both advanced treatment technologies when operating under optimized conditions achieved removal efficiencies of > 90% also for persistent micropollutants. Minimizing the pollution of reclaimed water thus met one relevant need for hydroponic lettuce cultivation.
Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Humanos , Hidroponía , Lactuca , Eliminación de Residuos Líquidos , Aguas Residuales , Agua , Contaminantes Químicos del Agua/análisisRESUMEN
In addition to analytical speciation, reliable Hg species modeling is crucial for predicting the mobility and toxicity of Hg, but geochemical speciation codes have not yet been tested for their prediction accuracy. Our study compares analyses of Hg species in highly Hg-contaminated groundwater (Hgtot: 0.02-4 µmol·L(-1)) at three sites with predictions of Hg speciation obtained from three geochemical codes (WHAM, Visual MINTEQ, PHREEQC) with and without implementation of Hg complexation by dissolved organic matter (DOM). Samples were analyzed for chemical composition, elemental, inorganic, and DOM-bound Hg (Hg(0), Hginorg, HgDOM). Hg-DOM complexation was modeled using three approaches: binding to humic/fulvic acids, binding to thiol-groups, or a combination of both. Results of Hg(0) modeling were poor in all scenarios. Prediction accuracy for Hginorg and HgDOM strongly depended on the assumed DOM composition. Best results were achieved when weaker binding sites, simulated by WHAMs DOM submodel, were combined with strongly binding thiol groups. Indications were found that thiol-DOM ratios in groundwater are likely to be lower than in surface water, highlighting the need for analytical thiol quantification in groundwater DOM. This study shows that DOM quality is a crucial parameter for prediction of Hg speciation in groundwater by means of geochemical modeling.
Asunto(s)
Agua Subterránea , Mercurio , Sustancias Húmicas , Agua/química , Contaminantes Químicos del AguaRESUMEN
Mercury (Hg) speciation and sorption analyses in contaminated aquifers are useful for understanding transformation, retention, and mobility of Hg in groundwater. In most aquifers hydrous ferric oxides (HFOs) are among the most important sorbents for trace metals; however, their role in sorption or mobilization of Hg in aquifers has been rarely analyzed. In this study, we investigated Hg chemistry and Hg sorption to HFO under changing redox conditions in a highly HgCl2-contaminated aquifer (up to 870µgL(-1) Hg). Results from aqueous and solid phase Hg measurements were compared to modeled (PHREEQC) data. Speciation analyses of dissolved mercury indicated that Hg(II) forms were reduced to Hg(0) under anoxic conditions, and adsorbed to or co-precipitated with HFO. Solid phase Hg thermo-desorption measurements revealed that between 55 and 93% of Hg bound to HFO was elemental Hg (Hg(0)). Hg concentrations in precipitates reached more than 4 weight %, up to 7000 times higher than predicted by geochemical models that do not consider unspecific sorption to and co-precipitation of elemental Hg with HFO. The observed process of Hg(II) reduction and Hg(0) formation, and its retention and co-precipitation by HFO is thought to be crucial in HgCl2-contaminated aquifers with variable redox-conditions regarding the related decrease in Hg solubility (factor of ~10(6)), and retention of Hg in the aquifer.