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PubMed2002

Biological hydrogen production measured in batch anaerobic respirometers.

The biological production of hydrogen from the fermentation of different substrates was examined in batch tests using heat-shocked mixed cultures with two techniques: an intermittent pressure release method (Owen method) and a continuous gas release method using a bubble measurement device (respirometric method). Under otherwise identical conditions, the respirometric method resulted in the production of 43% more hydrogen gas from glucose than the Owen method. The lower conversion of glucose to hydrogen using the Owen protocol may have been produced by repression of hydrogenase activity from high partial pressures in the gastight bottles, but this could not be proven using a thermodynamic/rate inhibition analysis. In the respirometric method, total pressure in the headspace never exceeded ambient pressure, and hydrogen typically composed as much as 62% of the headspace gas. High conversion efficiencies were consistently obtained with heat-shocked soils taken at different times and those stored for up to a month. Hydrogen gas composition was consistently in the range of 60-64% for glucose-grown cultures during logarithmic growth but declined in stationary cultures. Overall, hydrogen conversion efficiencies for glucose cultures were 23% based on the assumption of a maximum of 4 mol of hydrogen/ mol of glucose. Hydrogen conversion efficiencies were similar for sucrose (23%) and somewhat lower for molasses (15%) but were much lower for lactate (0.50%) and cellulose (0.075%).

Bacteria, Anaerobic↗
PubMed2002

Occurrence and destruction of PAHs, PCBs, CIPhs, CIBzs, and PCDD/Fs in ash from gasification of straw.

Two experiments were performed with an atmospheric circulating fluidized bed gasifier (ACFBG), the first with pelletized straw and the second with loose straw, to investigate the occurrence of polycyclic aromatic hydrocarbons (PAHs), chlorophenols (CIPhs), polychlorinated biphenyls (PCBs), polychlorinated benzenes (ClBzs), polychlorinated dibenzo-p-dioxins (PCDDs), and polychlorinated dibenzofurans (PCDFs) in the bottom ash and fly ash formed during gasification. Only PAHs were present in large amounts, and only in the fly ash, ranging from 300 to 555 mg/kg ash in the tests with pelletized straw and from 73 to 118 mg/kg ash in those with loose straw. These amounts are so high that environmentally safe disposal or reuse of the ash would be difficult, so the development of a technique to handle the problem was included in the project. The method investigated was to burn the fly ash in a circulating fluidized bed (CFB) boiler in order to destroy the PAHs. This worked surprisingly well, eliminating 99% of the PAHs, without any further formation of the other harmful organic compounds analyzed. Thus, this method could actually be useful in practice. Especially the fact that the formation of PCDD/Fs was minimal during gasification and further treatment of the ash in the CFB boiler makes the gasification technique highly competitive relative to conventional combustion methods.

Benzofurans↗
PubMed2003

The relative effectiveness of pH control and heat treatment for enhancing biohydrogen gas production.

Hydrogen gas can be recovered from the microbial fermentation of organic substrates at high concentrations when interspecies hydrogen transfer to methanogens is prevented. Two techniques that have been used to limit methanogenesis in mixed cultures are heat treatment, to remove nonsporeforming methanogens from an inoculum, and low pH during culture growth. We found that high hydrogen gas concentrations (57-72%) were produced in all tests and that heat treatment (HT) of the inoculum (pH 6.2 or 7.5) produced greater hydrogen yields than low pH (6.2) conditions with a nonheat-treated inoculum (NHT). Conversion efficiencies of glucose to hydrogen (based on a theoretical yield of 4 mol-H2/mol-glucose) were as follows: 24.2% (HT, pH = 6.2), 18.5% (HT, pH = 7.5), 14.9% (NHT, pH = 6.2), and 12.1% (NHT, pH = 7.5). The main products of glucose (3 g-COD/L) utilization (> or = 99%) in batch tests were acetate (3.4-24.1%), butyrate (6.4-29.4%), propionate (0.3-12.8%), ethanol (15.4-28.8%), and hydrogen (4.0-8.1%), with lesser amounts of acetone, propanol, and butanol (COD basis). Hydrogen gas phase concentrations in all batch cultures reached a maximum of 57-72% after 30 h but thereafter rapidly declined to nondetectable levels within 80 h. Separate experiments showed substantial hydrogen losses could occur via acetogenesis and that heat treatment did not prevent acetogenesis. Heat treatment consistently eliminated the production of measurable concentrations of methane. The disappearance of ethanol produced during hydrogen production was likely due to acetic acid production as thermodynamic calculations show that this reaction is spontaneous once hydrogen is depleted. Overall, these results show that low pH was, without heat treatment, sufficient to control hydrogen losses to methanogens in mixed batch cultures and suggest that methods will need to be found to limit acetogenesis in order to increase hydrogen gas yields by batch cultures.

Bacteria, Anaerobic↗
PubMed2004

Enhanced biohydrogen production from sewage sludge with alkaline pretreatment.

Batch tests were carried out to analyze influences of the alkaline pretreatment and initial pH value on biohydrogen production from sewage sludge. Experimental results of the impact of different initial pH on biohydrogen production showed that both the maximal hydrogen yield occurred and that no methane was detected in the tests of at the initial pH of 11.0. The final pH decreased at the initial pH of 7.0-12.5 but increased atthe initial pH of 3.0-6.0, probably due to the combination of solubilized protein from sludge and the formation of volatile fatty acids (VFAs) and ammonia during biohydrogen fermentation. The performance of biohydrogen production using the raw sludge and the alkaline pretreated sludge was then compared in batch fermentation tests atthe initial pH of 11.0. The hydrogen yield was increased from 9.1 mL of H2/g of dry solids (DS) of the raw sludge to 16.6 mL of H2/g of DS of the alkaline pretreated sludge. No methane and less carbon dioxide (0.8% of control) were present in the biohydrogen production from the alkaline pretreated sludge. These results clearly showed that biohydrogen production could be enhanced and maintained stable by the combination of the high initial pH and alkaline pretreatment. The mechanism of biohydrogen production from sewage sludge at high initial pH was therefore investigated because the results of this study were differentfrom previous studies of biohydrogen production. Results showed that protein was the major substrate for biohydrogen production from sewage sludge and that Eubacterium multiforme and Paenibacillus polymyxa were the dominant bacteria in biohydrogen production from alkaline pretreated sludge at an initial pH of 11.0. The combination of alkaline pretreatment and high initial pH could not only maintain a suitable pH range for the growth of dominant hydrogen-producing anaerobes but also inhibit the growth of hydrogen-consuming anaerobes. In addition, the changes in pH value, oxidation-reduction potential, VFAs and soluble COD during hydrogen fermentation were also discussed.

Bioelectric Energy Sources↗
PubMed2004

Production of electricity during wastewater treatment using a single chamber microbial fuel cell.

Microbial fuel cells (MFCs) have been used to produce electricity from different compounds, including acetate, lactate, and glucose. We demonstrate here that it is also possible to produce electricity in a MFC from domestic wastewater, while atthe same time accomplishing biological wastewater treatment (removal of chemical oxygen demand; COD). Tests were conducted using a single chamber microbial fuel cell (SCMFC) containing eight graphite electrodes (anodes) and a single air cathode. The system was operated under continuous flow conditions with primary clarifier effluent obtained from a local wastewater treatment plant. The prototype SCMFC reactor generated electrical power (maximum of 26 mW m(-2)) while removing up to 80% of the COD of the wastewater. Power output was proportional to the hydraulic retention time over a range of 3-33 h and to the influent wastewater strength over a range of 50-220 mg/L of COD. Current generation was controlled primarily by the efficiency of the cathode. Optimal cathode performance was obtained by allowing passive air flow rather than forced air flow (4.5-5.5 L/min). The Coulombic efficiency of the system, based on COD removal and current generation, was < 12% indicating a substantial fraction of the organic matter was lost without current generation. Bioreactors based on power generation in MFCs may represent a completely new approach to wastewater treatment. If power generation in these systems can be increased, MFC technology may provide a new method to offset wastewater treatment plant operating costs, making advanced wastewater treatment more affordable for both developing and industrialized nations.

Bioelectric Energy Sources↗
PubMed2005

Microbial fuel cell using anaerobic respiration as an anodic reaction and biomineralized manganese as a cathodic reactant.

We have operated a microbial fuel cell in which glucose was oxidized by Klebsiella pneumoniae in the anodic compartment, and biomineralized manganese oxides, deposited by Leptothrix discophora, were electrochemically reduced in the cathodic compartment. In the anodic compartment, to facilitate the electron transfer from glucose to the graphite electrode, we added a redox mediator, 2-hydroxy-1,4-naphthoquinone. We did not add any redox mediator to the cathodic compartment because the biomineralized manganese oxides were deposited on the surface of a graphite electrode and were reduced directly by electrons from the electrode. We have demonstrated that biomineralized manganese oxides are superiorto oxygen when used as cathodic reactants in microbial fuel cells. The current density delivered by using biomineralized manganese oxides as the cathodic reactant was almost 2 orders of magnitude higher than that delivered using oxygen. Several fuel cells were operated for 500 h, reaching anodic potentials of -441.5 +/- 31 mVscE and cathodic potentials of +384.5 +/- 64 mVscE. When the electrodes were connected by a 50 Ohms resistor, the fuel cell delivered the peak power density of 126.7 +/- 31.5 mW/m2.

Bioelectric Energy Sources↗
PubMed2005

Microbial phenazine production enhances electron transfer in biofuel cells.

High-rate electron transfer toward an anode in microbial fuel cells (MFCs) has thus far not been described for bacteria-producing soluble redox mediators. To studythe mechanism of electron transfer, we used a MFC isolate, Pseudomonas aeruginosa strain KRP1. Bacterial electron transfer toward the MFC anode was enabled through pyocyanin and phenazine-1-carboxamide. The presence of the anode stimulated pyocyanin production. Mutant strains, deficient in the synthesis of pyocyanin and phenazine-1-carboxamide, were unable to achieve substantial electron transfer and reached only 5% of the wild type's power output. Upon pyocyanin addition, the power output was restored to 50%. Pyocyanin was not only used by P. aeruginosa to improve electron transfer but as well enhanced electron transfer by other bacterial species. The finding that one bacterium can produce electron shuttles, which can be used also by other bacteria, to enhance electron-transfer rate and growth, has not been shown before. These findings have considerable implications with respect to the power output attainable in MFCs.

Bioelectric Energy Sources↗
PubMed2005

Production of electricity from acetate or butyrate using a single-chamber microbial fuel cell.

Hydrogen can be recovered by fermentation of organic material rich in carbohydrates, but much of the organic matter remains in the form of acetate and butyrate. An alternative to methane production from this organic matter is the direct generation of electricity in a microbial fuel cell (MFC). Electricity generation using a single-chambered MFC was examined using acetate or butyrate. Power generated with acetate (800 mg/L) (506 mW/m2 or 12.7 mW/ L) was up to 66% higher than that fed with butyrate (1000 mg/L) (305 mW/m2 or 7.6 mW/L), demonstrating that acetate is a preferred aqueous substrate for electricity generation in MFCs. Power output as a function of substrate concentration was well described by saturation kinetics, although maximum power densities varied with the circuit load. Maximum power densities and half-saturation constants were Pmax = 661 mW/m2 and Ks = 141 mg/L for acetate (218 ohms) and Pmax = 349 mW/m2 and Ks = 93 mg/L for butyrate (1000 ohms). Similar open circuit potentials were obtained in using acetate (798 mV) or butyrate (795 mV). Current densities measured for stable power outputwere higher for acetate (2.2 A/m2) than those measured in MFCs using butyrate (0.77 A/m2). Cyclic voltammograms suggested that the main mechanism of power production in these batch tests was by direct transfer of electrons to the electrode by bacteria growing on the electrode and not by bacteria-produced mediators. Coulombic efficiencies and overall energy recovery were 10-31 and 3-7% for acetate and 8-15 and 2-5% for butyrate, indicating substantial electron and energy losses to processes other than electricity generation. These results demonstrate that electricity generation is possible from soluble fermentation end products such as acetate and butyrate, but energy recoveries should be increased to improve the overall process performance.

Acetates↗
PubMed2004

Continuous electricity generation from domestic wastewater and organic substrates in a flat plate microbial fuel cell.

A microbial fuel cell (MFC) is a device that converts organic matter to electricity using microorganisms as the biocatalyst. Most MFCs contain two electrodes separated into one or two chambers that are operated as a completely mixed reactor. In this study, a flat plate MFC (FPMFC) was designed to operate as a plug flow reactor (no mixing) using a combined electrode/proton exchange membrane (PEM) system. The reactor consisted of a single channel formed between two nonconductive plates that were separated into two halves by the electrode/PEM assembly. Each electrode was placed on an opposite side of the PEM, with the anode facing the chamber containing the liquid phase and the cathode facing a chamber containing only air. Electricity generation using the FPMFC was examined by continuously feeding a solution containing wastewater, or a specific substrate, into the anode chamber. The system was initially acclimated for 1 month using domestic wastewater orwastewater enriched with a specific substrate such as acetate. Average power density using only domestic wastewater was 72+/-1 mW/m2 at a liquid flow rate of 0.39 mL/min [42% COD (chemical oxygen demand) removal, 1.1 h HRT (hydraulic retention time)]. At a longer HRT = 4.0 h, there was 79% COD removal and an average power density of 43+/-1 mW/m2. Power output was found to be a function of wastewater strength according to a Monod-type relationship, with a half-saturation constant of Ks = 461 or 719 mg COD/L. Power generation was sustained at high rates with several organic substrates (all at approximately 1000 mg COD/L), including glucose (212+/-2 mW/ m2), acetate (286+/-3 mW/m2), butyrate (220+/-1 mW/ m2), dextran (150+/-1 mW/m2), and starch (242+/-3 mW/ m2). These results demonstrate the versatility of power generation in a MFC with a variety of organic substrates and show that power can be generated at a high rate in a continuous flow reactor system.

Bioelectric Energy Sources↗
PubMed2004

Cathode performance as a factor in electricity generation in microbial fuel cells.

Although microbial fuel cells (MFCs) generate much lower power densities than hydrogen fuel cells, the characteristics of the cathode can also substantially affect electricity generation. Cathodes used for MFCs are often either Pt-coated carbon electrodes immersed in water that use dissolved oxygen as the electron acceptor or they are plain carbon electrodes in a ferricyanide solution. The characteristics and performance of these two cathodes were compared using a two-chambered MFC. Power generation using the Pt-carbon cathode and dissolved oxygen (saturated) reached a maximum of 0.097 mW within 120 h after inoculation (wastewater sludge and 20 mM acetate) when the cathode was equal size to the anode (2.5 x 4.5 cm). Once stable power was generated after replacing the MFC with fresh medium (no sludge), the Coulombic efficiency ranged from 63 to 78%. Power was proportional to the dissolved oxygen concentration in a manner consistent with Monod-type kinetics, with a half saturation constant of K(DO) = 1.74 mg of O2/L. Power increased by 24% when the cathode surface areas were increased from 22.5 to 67.5 cm2 and decreased by 56% when the cathode surface area was reduced to 5.8 cm2. Power was also substantially reduced (by 78% to 0.02 mW) if Pt was not used on the cathode. By using ferricyanide instead of dissolved oxygen, the maximum power increased by 50-80% versus that obtained with dissolved oxygen. This result was primarily due to increased mass transfer efficiencies and the larger cathode potential (332 mV) of ferricyanide than that obtained with dissolved oxygen (268 mV). A cathode potential of 804 mV (NHE basis) is theoretically possible using dissolved oxygen, indicating that further improvements in cathode performance with oxygen as the electron acceptor are possible that could lead to increased power densities in this type of MFC.

Bioelectric Energy Sources↗
PubMed2005

Hygroscopicity of water-soluble organic compounds in atmospheric aerosols: amino acids and biomass burning derived organic species.

Amino acids and organic species derived from biomass burning can potentially affect the hygroscopicity and cloud condensation activities of aerosols. The hygroscopicity of seven amino acids (glycine, alanine, serine, glutamine, threonine, arginine, and asparagine) and three organic species most commonly detected in biomass burning aerosols (levoglucosan, mannosan, and galactosan) were measured using an electrodynamic balance. Crystallization was observed in the glycine, alanine, serine, glutamine, and threonine particles upon evaporation of water, while no phase transition was observed in the arginine and asparagine particles even at 5% relative humidity (RH). Water activity data from these aqueous amino acid particles, except arginine and asparagine, was used to revise the interaction parameters in UNIQUAC functional group activity coefficients to give predictions to within 15% of the measurements. Levoglucosan, mannosan, and galactosan particles did not crystallize nor did they deliquesce. They existed as highly concentrated liquid droplets at low RH, suggesting that biomass burning aerosols retain water at low RH. In addition, these particles follow a very similar pattern in hygroscopic growth. A generalized growth law (Gf = (1 - RH/100)-0.095) is proposed for levoglucosan, mannosan, and galactosan particles.

Aerosols↗
PubMed2004

Electricity generation using an air-cathode single chamber microbial fuel cell in the presence and absence of a proton exchange membrane.

Microbial fuel cells (MFCs) are typically designed as a two-chamber system with the bacteria in the anode chamber separated from the cathode chamber by a polymeric proton exchange membrane (PEM). Most MFCs use aqueous cathodes where water is bubbled with air to provide dissolved oxygen to electrode. To increase energy output and reduce the cost of MFCs, we examined power generation in an air-cathode MFC containing carbon electrodes in the presence and absence of a polymeric proton exchange membrane (PEM). Bacteria present in domestic wastewater were used as the biocatalyst, and glucose and wastewater were tested as substrates. Power density was found to be much greater than typically reported for aqueous-cathode MFCs, reaching a maximum of 262 +/- 10 mW/m2 (6.6 +/- 0.3 mW/L; liquid volume) using glucose. Removing the PEM increased the maximum power density to 494 +/- 21 mW/m2 (12.5 +/- 0.5 mW/L). Coulombic efficiency was 40-55% with the PEM and 9-12% with the PEM removed, indicating substantial oxygen diffusion into the anode chamber in the absence of the PEM. Power output increased with glucose concentration according to saturation-type kinetics, with a half saturation constant of 79 mg/L with the PEM-MFC and 103 mg/L in the MFC without a PEM (1000 omega resistor). Similar results on the effect of the PEM on power density were found using wastewater, where 28 +/- 3 mW/m2 (0.7 +/- 0.1 mW/L) (28% Coulombic efficiency) was produced with the PEM, and 146 +/- 8 mW/m2 (3.7 +/- 0.2 mW/L) (20% Coulombic efficiency) was produced when the PEM was removed. The increase in power output when a PEM was removed was attributed to a higher cathode potential as shown by an increase in the open circuit potential. An analysis based on available anode surface area and maximum bacterial growth rates suggests that mediatorless MFCs may have an upper order-of-magnitude limit in power density of 10(3) mW/m2. A cost-effective approach to achieving power densities in this range will likely require systems that do not contain a polymeric PEM in the MFC and systems based on direct oxygen transfer to a carbon cathode.

Bacteria↗
PubMed2005

Electrochemically assisted microbial production of hydrogen from acetate.

Hydrogen production via bacterial fermentation is currently limited to a maximum of 4 moles of hydrogen per mole of glucose, and under these conditions results in a fermentation end product (acetate; 2 mol/mol glucose) that bacteria are unable to further convert to hydrogen. It is shown here that this biochemical barrier can be circumvented by generating hydrogen gas from acetate using a completely anaerobic microbial fuel cell (MFC). By augmenting the electrochemical potential achieved by bacteria in this MFC with an additional voltage of 250 mV or more, it was possible to produce hydrogen at the cathode directly from the oxidized organic matter. More than 90% of the protons and electrons produced by the bacteria from the oxidation of acetate were recovered as hydrogen gas, with an overall Coulombic efficiency (total recovery of electrons from acetate) of 60-78%. This is equivalent to an overall yield of 2.9 mol H2/mol acetate (assuming 78% Coulombic efficiency and 92% recovery of electrons as hydrogen). This bio-electrochemically assisted microbial system, if combined with hydrogen fermentation that produces 2-3 mol H2/mol glucose, has the potential to produce ca. 8-9 mol H2/mol glucose at an energy cost equivalent to 1.2 mol H2/mol glucose. Production of hydrogen by this anaerobic MFC process is not limited to carbohydrates, as in a fermentation process, as any biodegradable dissolved organic matter can theoretically be used in this process to generate hydrogen from the complete oxidation of organic matter.

Acetates↗
PubMed2005

Electricity generation from artificial wastewater using an upflow microbial fuel cell.

The upflow microbial fuel cell (UMFC) was developed to generate electricity while simultaneously treating wastewater. During a five-month period of feeding a sucrose solution as the electron donor, the UMFC continuously generated electricity with a maximum power density of 170 mW/m2. To achieve this power density, the artificial electron-mediator hexacyanoferrate was required in the cathode chamber. The power density increased with increasing chemical oxygen demand (COD) loading rates up to 2.0 g COD/ L/day after which no further increases in power density were observed, indicating the presence of limiting factors. The overarching limiting factor for the UMFC in this study was the internal resistance, which was estimated as 84 omega at the maximum power density, and restricted the power output by causing a significant decrease in operating potential. Low Coulombic efficiencies varying from 0.7 to 8.1% implied that the electron-transfer bacteria were incapable of converting all of the available organics into electricity, so the excessive substrate created niches for the growth of methanogens. We found that the soluble COD (SCOD) removal efficiencies remained over 90% throughout the operational period, mainly because of methanogenic activity, which accounted for 35 to 58% of the SCOD removed at a loading rate of 1.0 g COD/L/ day. Additionally, transport limitation due to insufficient substrate diffusion was shown by cyclic voltammetry (CV).

Bacteria↗