In situ bioremediation of industrial chlorinated solvents, such as trichloroethene (TCE), is typically accomplished by providing an organic electron donor to naturally occurring dechlorinating populations. In the present study, we show that TCE dechlorinating bacteria can access the electrons required for TCE dechlorination directly from a negatively polarized (-450 mV vs. SHE) carbon paper electrode. In replicated batch experiments, a mixed dechlorinating culture, also containing Dehalococcoides spp., dechlorinated TCE to cis-dichloroethene (cis-DCE) and lower amounts of vinyl chloride (VC) and ethene using the polarized electrode as the sole electron donor. Conversely, neither VC nor ethene formation occurred when a pure culture of the electro-active microorganism Geobacter lovleyi was used, under identical experimental conditions. Cyclic voltammetry tests, carried out on the filter-sterilized supernatant of the mixed culture revealed the presence of a self-produced redox mediator, exhibiting a midpoint potential of around -400 mV (vs. SHE). This yet unidentified redox-active molecule appeared to be involved in the extracellular electron transfer from the electrode to the dechlorinating bacteria. The ability of dechlorinating bacteria to use electrodes as electron donors opens new perspectives for the development of clean, versatile, and efficient bioremediation systems based on a controlled subsurface delivery of electrons in support of biodegradative metabolisms and provides further evidence on the possibility of using conductive materials to manipulate and control a range of microbial bioprocesses.
Recently,the proof-of-principle of an innovative bioelectrochemical process fortrichloroethene (TCE) bioremediation was presented. In this newly developed process, a solid-state electrode polarized to -450 mV (vs SHE), in the presence of a low-potential redox mediator (methyl viologen), is employed as an electron donor for the microbial reductive dechlorination of TCE to lower or nonchlorinated end products. In the present study, we investigated the influence of methyl viologen and TCE concentrations on process performance. Using a highly enriched hydrogenotrophic dechlorinating culture, as a source culture in batch experiments, we found that TCE dechlorination and H2 evolution were the two main biological reactions which were stimulated. The relative contribution of the two reactions appeared to be strongly dependent on the mediator concentration. At the lowest methyl viologen (MV) concentrations (25-750 microM), only TCE dechlorination was stimulated, and no H2 was produced; at higher MV concentrations, both reactions occurred simultaneously, although they showed distinct kinetic features. In batch experiments in which TCE was omitted from the system, the rate of H2 production was remarkably increased (up to 80 times), suggesting that protons represented an alternative electron sink in the absence of the more energetically favorable TCE. Clearly, optimization of the process for TCE dechlorination requires H2 evolution to be minimized by, for instance, operating the system at low mediator concentrations, and this can be possibly achieved through proper physical immobilization of the mediator at the electrode surface. On the other hand, the observed bioelectrocatalytic H2 production occurred at virtually no overpotentials with respect to the thermodynamic 2H+/H2 potential. This finding revealed that the dechlorinating culture employed represented quite an exceptional and previously unrecognized biocatalytic system for H2 production.
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