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Perfluoroalkyl and polyfluoroalkyl substances (PFASs) represent hazardous pollutants and are frequently detected in the environment, e.g. in contaminated groundwater. PFASs are persistent to biodegradation and conventional oxidation processes such as ozonation. In this study electrochemical degradation of PFASs on boron-doped diamond (BDD) electrodes is demonstrated. Experiments were performed with model solutions and contaminated groundwater with a dissolved organic carbon (DOC) content of 13 mg/L. The perfluorinated carboxylic acids (PFCAs) perfluorobutanoate, perfluoropentanoate, perfluorohexanoate, perfluoroheptanoate and perfluorooctanoate, and the perfluorinated sulfonic acids (PFSAs) perfluorobutane sulfonate, perfluorohexane sulfonate, perfluorooctane sulfonate and 6:2 fluorotelomer sulfonate were detected in the groundwater samples. At PFAS concentrations ranging from 0.26 to 34 mg/L (0.7 to 79 μM), the degradation of PFASs was achieved despite of the high DOC background. Pseudo first-order kinetic constants of PFSA degradation increased with the increase of carbon chain length. Fluoride formation as well as the generation of PFCAs with shortened chain lengths was observed. Inorganic byproducts such as perchlorate were also formed and have to be considered in further process optimization.

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This article for the first time demonstrates successful application of electrochemical processes to stimulate sequential reductive/oxidative microbial degradation of perchloroethene (PCE) in mineral medium and in contaminated groundwater. In a flow-through column system, hydrogen generation at the cathode supported reductive dechlorination of PCE to cis-dichloroethene (cDCE), vinyl chloride (VC), and ethene (ETH). Electrolytically generated oxygen at the anode allowed subsequent oxidative degradation of the lower chlorinated metabolites. Aerobic cometabolic degradation of cDCE proved to be the bottleneck for complete metabolite elimination. Total removal of chloroethenes was demonstrated for a PCE load of approximately 1.5 μmol/d. In mineral medium, long-term operation with stainless steel electrodes was demonstrated for more than 300 days. In contaminated groundwater, corrosion of the stainless steel anode occurred, whereas DSA (dimensionally stable anodes) proved to be stable. Precipitation of calcareous deposits was observed at the cathode, resulting in a higher voltage demand and reduced dechlorination activity. With DSA and groundwater from a contaminated site, complete degradation of chloroethenes in groundwater was obtained for two months thus demonstrating the feasibility of the sequential bioelectro-approach for field application.

Bioelectrochemical systems (BESs) are hybrid systems using electroactive bacteria and solid electrodes, which serve as electron donor or acceptor for microorganisms. When forming a biofilm on the electrode, bacteria secrete extracellular polymeric substances (EPSs). However, EPS excretion of electroactive biofilms in BES has been rarely studied so far. Consequently, the aim of this study is to develop a routine including the electrochemical cultivation, biofilm harvesting, fractionation, and biochemical analysis of the EPS secreted by Geobacter sulfurreducens under electroactive conditions. G. sulfurreducens was cultivated in microbial fuel cell mode on graphite-based electrodes polarized to +400 mV versus Ag/AgCl for 8 d. A maximum current density of 172 ± 29 μA cm–2 was reached after 7 d. The EPS secreted from the biofilms were harvested and fractioned into soluble, loosely bound, and tightly bound EPS and biochemically analyzed. Electroactive cultures secreted significantly more EPSs compared to cells grown under standard heterotrophic conditions (fumarate respiration). With 116 pg per cell, the highest amount of EPSs was measured for the soluble EPS fraction of G. sulfurreducens using anodic respiration, followed by the tightly bound (18 pg cell–1) and loosely bound (11 pg cell–1) fractions of the EPS. Proteins were found to dominate all EPS fractions of the biofilms grown under electrochemical conditions. To the best of the authors’ knowledge, these experiments are the first approach toward a complete analysis of the main EPS components of G. sulfurreducens under anode-respiring conditions.

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