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Bioelectrochemical system is an emerging technology for the remediation of soils contaminated by petroleum hydrocarbons. However, performance of such systems can be limited by the inefficient mass transport in soil. Here we report a new method of sand amendment, which significantly increases both oxygen and proton transports, resulting to increased soil porosity (from 44.5% to 51.3%), decreased Ohmic resistance (by 46%), and increased charge output (from 2.5 to 3.5Cg(-1)soil). The degradation rates of petroleum hydrocarbons increased by up to 268% in 135d. The degradation of n-alkanes and polycyclic aromatic hydrocarbons with high molecular weight was accelerated, and denaturing gradient gel electrophoresis showed that the microbial community close to the air-cathode was substantially stimulated by the induced current, especially the hydrocarbon degrading bacteria Alcanivorax. The bioelectrochemical stimulation imposed a selective pressure on the microbial community of anodes, including that far from the cathode. These results suggested that sand amendment can be an effective approach for soil conditioning that will enhances the bioelectrochemical removal of hydrocarbons in contaminated soils.

BACKGROUND: Bioelectrochemical remediation of soils contaminated by petroleum hydrocarbons has received increasing attention as an effective approach to remove pollution with simultaneous electricity generation. RESULTS: Here, glucose was added as a co-substrate in this system. The charge output of soil microbial fuel cells (MFCs) was enhanced by 262%, and the total petroleum hydrocarbon degradation rate increased by 200%. According to the increased dehydrogenase and polyphenol oxidase activities, the exogenetic glucose substantially activated hydrocarbon degradation bacteria (such as Alcanivorax). The Shannon–Wiener Index and richness of soil microbial community decreased after glucose addition, indicating that a selective enrichment of specific communities was imposed by glucose. Correlation analysis showed the biodiversity in soil far from the cathode was mainly determined by the concentration of petroleum hydrocarbons, while that in soil close to the cathode was dominated by the current. CONCLUSION: This study demonstrated that an exogenetic carbon source enhanced the bioelectrochemically assisted degradation of aged petroleum hydrocarbons in saline soils, providing an effective approach to remove contaminations from soil in barren areas or extreme environments. © 2015 Society of Chemical Industry Supporting information may be found in the online version of this article.

Here, we report a new microbial electrolysis cell (MEC) system for hydrogen generation that was composed of a microbial fuel cell (MFC) and a bio-photoelectrochemical cell (BPEC). The BPEC consisted of a photocathode and a microbially-catalyzed anode. In the new MEC system, hydrogen was produced by the BPEC photocathode when it was illuminated with visible light, with the voltage for electrolysis supplied by the MFC. The electrons produced from the MFC anode were transferred to the BPEC photocathode through an external circuit and then photogenerated holes captured some of the electrons emitted by the MFC anode under visible light. This prevented the recombination of the photogenerated hole and electron pairs, leaving more photogenerated electrons available for hydrogen evolution reactions. This also allowed the remaining electrons from the MFC anode to participate in hydrogen evolution reactions. Under visible light, hydrogen was continuously produced from the new MEC system, with a maximum current density of 0.68 A m−2 and an average hydrogen-production rate of 1.35 ± 0.15 mL h−1.

With the aim of in situ bioremediation of soil contaminated by hydrocarbons, anodes arranged with two different ways (horizontal or vertical) were compared in microbial fuel cells (MFCs). Charge outputs as high as 833 and 762C were achieved in reactors with anodes horizontally arranged (HA) and vertically arranged (VA). Up to 12.5 % of the total petroleum hydrocarbon (TPH) was removed in HA after 135 days, which was 50.6 % higher than that in VA (8.3 %) and 95.3 % higher than that in the disconnected control (6.4 %). Hydrocarbon fingerprint analysis showed that the degradation rates of both alkanes and polycyclic aromatic hydrocarbons (PAHs) in HA were higher than those in VA. Lower mass transport resistance in the HA than that of the VA seems to result in more power and more TPH degradation. Soil pH was increased from 8.26 to 9.12 in HA and from 8.26 to 8.64 in VA, whereas the conductivity was decreased from 1.99 to 1.54 mS/cm in HA and from 1.99 to 1.46 mS/cm in VA accompanied with the removal of TPH. Considering both enhanced biodegradation of hydrocarbon and generation of charge in HA, the MFC with anodes horizontally arranged is a promising configuration for future applications.

Bioelectrochemical remediation is an emerging technology for in situ removal of petroleum hydrocarbons in soil. Here we demonstrated that the remediation can be extended to a larger range by adding multilayer anodes in contaminated soils. Using a three anodes system with activated carbon as the cathodic catalyst, 918 C of charge transferred during 180 days in aged saline soil. The degradation of both polycyclic aromatic hydrocarbons (PAHs) and n-alkanes were accelerated in each layer compared to the disconnected control. The net degradation rates of total petroleum hydrocarbons, 16 priority PAHs and total n-alkanes (C8–C40) were 18%, 36% and 29%, respectively. Popular exoelectrogens (such as Geobacteraceae sp.) and Escherichia were identified, which possibly played an important role in this bioelectrochemical process.

The extreme salinity and high internal resistance of saline-alkali soil contaminated by petroleum hydrocarbons were two key limitations for using the bioelectrochemical remediation. In order to solve two problems, we simply rinsed soil, added carbon fiber to polluted soil. The charge output was enhanced by 110% with increase of the maximum current densities from 81 to 304 mA·m−2 while hydrocarbons degradation rate enhanced by 484%, especially the high molecular weight fractions (C28–C36 of n-alkanes and 4–6 rings of PAHs). These effects were possibly due to the selective enrichment of species belonged to δ-Proteobacteria (Proteobacteria), Flavobacteriia (Bacteroidetes) or Clostridia (Firmicutes), the activities of biological electron transfer and enzymes. As we know, oxygenase gene that directly decided the process of degradation, was surveyed for the first time in soil bioelectrochemical remediation system. The results confirmed that the bio-current stimulated the activities of naphthalene dioxygenase and xylene monooxygenase and thus the hydrocarbons degradation and the electricity generation. Given that electricity generation and the remediation performance are governed by multiple factors, understanding of microbial community and enzyme gene is crucial to promote the power yield and the bioelectrochemical remediation applicability.

Activated carbon (AC) is a promising catalyst for the air cathode of microbial fuel cells (MFCs) because of its high performance and low cost. To increase the performance of AC air cathodes, the acceleration of OH(-) transport is one of the most important methods, but it has not been widely investigated. Here we added quaternary ammonium to ACs by in situ anchoring of a quaternary ammonium/epoxide-reacting compound (QAE) or ex situ mixing with anion exchange resins in order to modify ACs from not only the external surface but also inside the pores. In 50 mM phosphate buffer solution (PBS), the in situ anchoring of QAE was a more effective way to increase the power. The highest power density of 2781 ± 36 mW/m(2), which is 10% higher than that of the control, was obtained using QAE-anchored AC cathodes. When the medium was switched to an unbuffered NaCl solution, the increase in maximum power density (885 ± 25 mW/m(2)) was in accordance with the anion exchange capacity (0.219 mmol/g). The highest power density of the anion exchange resin-mixed air cathode was 51% higher than that of the control, indicating that anion exchange is urgently needed in real wastewaters. Excess anchoring of QAE blocked both the mesopores and micropores, causing the power output to be inhibited.

The electrical conductivity (EC) of soil is generally measured after soil extraction, so this method cannot represent the in situ EC of soil (e.g., EC of soils with different moisture contents) and therefore lacks comparability in some cases. Using a resistance measurement apparatus converted from a configuration of soil microbial fuel cell, the in situ soil EC was evaluated according to the Ohmic resistance (Rs) measured using electrochemical impedance spectroscopy. The EC of soils with moisture content from 9.1% to 37.5% was calculated according to Rs. A significant positive correlation (R2 = 0.896, p < 0.01) between the soil EC and the moisture content was observed, which demonstrated the feasibility of the approach. This new method can not only represent the actual soil EC, but also does not need any pretreatment. Thus it may be used widely in the measurement of the EC for soils and sediments.