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PubMed2006

Two-phase anaerobic digestion for production of hydrogen-methane mixtures.

An anaerobic digestion process to produce hydrogen and methane in two sequential stages was investigated, using two bioreactors of 2 and 15 L working volume, respectively. This relative volume ratio (and shorter retention time in the second, CH(4)-producing reactor) was selected, in part, to test the assumption that separation of phase can enhance metabolism in the second methane producing reactor. The reactor system was seeded with conventional anaerobic digester sludge, fed with a glucose-yeast extract--peptone medium and operated under conditions of relatively low mixing, to simulate full scale operation. A total of nine steady states were investigated, spanning a range of feed concentrations, dilution rates, feed carbon to nitrogen ratios and degree of integration of the two stages. The performance of this two-stage process and potential practical applications for the production of clean-burning hydrogen-methane mixtures are discussed.

Bacteria, Anaerobic↗

PubMed2005

Methane production and consumption in an active volcanic environment of Southern Italy.

Methane fluxes were measured, using closed chambers, in the Crater of Solfatara volcano, Campi Flegrei (Southern Italy), along eight transects covering areas of the crater presenting different landscape physiognomies. These included open bare areas, presenting high geothermal fluxes, and areas covered by vegetation, which developed along a gradient from the central open area outwards, in the form of maquis, grassland and woodland. Methane fluxes decreased logarithmically (from 150 to -4.5 mg CH4 m(-2)day(-1)) going from the central part of the crater (fangaia) to the forested edges, similarly to the CO2 fluxes (from 1500 g CO2 m(-2)day(-1) in the centre of the crater to almost zero flux in the woodlands). In areas characterized by high emissions, soil presented elevated temperature (up to 70 degrees C at 0-10 cm depth) and extremely low pH (down to 1.8). Conversely, in woodland areas pH was higher (between 3.7 and 5.1) and soil temperature close to air values. Soil (0-10 cm) was sampled, in two different occasions, along the eight transects, and was tested for methane oxidation capacity in laboratory. Areas covered by vegetation mostly consumed CH4 in the following order woodland>macchia>grassland. Methanotrophic activity was also measured in soil from the open bare area. Oxidation rates were comparable to those measured in the plant covered areas and were significantly correlated with field CH4 emissions. The biological mechanism of uptake was demonstrated by the absence of activity in autoclaved replicates. Thus results suggest the existence of a population of micro-organisms adapted to this extreme environment, which are able to oxidize CH4 and whose activity could be stimulated and supported by elevated concentrations of CH4.

Air Pollutants↗

PubMed2004

Surface properties and catalytic performance of La(1-x)Sr(x)FeO(3) perovskite-type oxides for methane combustion.

La(1-x)Sr(x)FeO(3) (x=0.0-1.0) perovskites were prepared and tested for the combustion of methane. X-ray diffraction (XRD) patterns revealed the presence of a single perovskite structure for substitutions 0x0.3, however Fe(2)O(3), SrCO(3) and SrFeO(3) phases were observed for substitutions x>0.3. The results of activity test indicate that with La(1-x)Sr(x)FeO(3) as the catalyst, the combustion of methane can take place at low temperatures around 400 degrees C. Partial substitution of La with Sr increases the activity and an optimal substitution fraction (x=0.5) exists in the La(1-x)Sr(x)FeO(3) catalysts. Catalyst activity can be well correlated to the product of the specific surface area and atomic ratio of Fe to La+Sr on the catalyst surface. Experimental results of O(2)-TPD and CH(4)-TPD in the range of 350-500 degrees C indicate that the amount of oxygen desorbed from the La(1-x)Sr(x)FeO(3) catalysts is far larger than that of methane. Therefore, it can be proposed that the catalytic oxidation of CH(4) over these catalysts proceeds with the surface reaction between CH(4) in the gas phase and the adsorbed O(2). Addition of water vapor or CO(2) to the feed inhibited catalyst activity, but the inhibition was reversible and became negligible at high reaction temperature.

Calcium Compounds↗

PubMed2005

Biogeochemical distinction of methane releases from two Amazon hydroreservoirs.

Biogeochemical distinction of methane emissions to the atmosphere may essentially rely on the surface area and morphometry of Amazon hydroreservoirs. Tucurui (deep) and Samuel (shallow) reservoirs released in average 13.82+/-22.94 and 71.19+/-107.4 mg CH4 m(-2)d(-1), respectively. delta13C-CH4 values from the sediments to the atmosphere indicate that the deep reservoir has extended methanotrophic layer, oxidizing large quantities of light isotope methane coming from the sediments, while sediment-generated methane can easily evade the shallow reservoir.

Atmosphere↗

PubMed2005

Methyl-coenzyme M reductase and the anaerobic oxidation of methane in methanotrophic Archaea.

Recent biochemical and metagenomic data indicate that not yet cultured Archaea that are closely related to methanogenic Archaea of the order of Methanosarcinales are involved in the anaerobic oxidation of methane in marine sediments. The DNA from the methanotrophic Archaea has been shown to harbor gene homologues for methyl-coenzyme M reductase, which in methanogenic Archaea catalyses the methane-forming reaction. In microbial mats catalyzing anaerobic oxidation of methane, this nickel enzyme has been shown to be present in concentrations of up to 10% of the total extracted proteins.

Anaerobiosis↗

PubMed2006

New improvements in methane detection using a Helmholtz resonant photoacoustic laser sensor: a comparison between near-IR diode lasers and mid-IR quantum cascade lasers.

Atmospheric methane was detected by combining a photoacoustic (PA) sensor with several lasers emitting in both the near- and mid-infrared spectral ranges to check the achievable detection limits. The PA spectrometer is based on differential Helmholtz resonance. Near-infrared telecommunication-type laser diodes of increasing power, from Sensors Unlimited Inc. and Anritsu, were first used to scan the 2 nu(3) band of CH(4) near 1.65 microm. The best achieved detection limit is 0.15 ppm of methane at atmospheric pressure and with a 1s integration time. The PA sensor was then operated in conjunction with a quantum cascade laser from Alpes Lasers emitting near 7.9 microm on the nu(4) band of CH(4). The achieved detection limit is then of 3 ppb. The dramatic improvement in the detection limit obtained with the QC laser is due to the stronger optical power as well as to the capability of reaching the fundamental bands of methane lying in the mid-infrared spectral range.

Acoustics↗

PubMed2004

Ensilage of pineapple processing waste for methane generation.

Pineapple peel wastes, which are seasonal, comprise of peels and rags. Their disposal poses a serious environmental pollution problem. Since pineapple peel is rich in cellulose, hemicellulose and other carbohydrates it was found to be a potential substrate for methane generation by anaerobic digestion. Ensilaging of pineapple peel resulted in the conversion of 55% carbohydrates into volatile fatty acids. The ensilage of pineapple processing wastes reduced the biological oxygen demand by 91%. Biogas digester fed with ensilaged pineapple peel resulted in the biogas yield of 0.67 m3/kg volatile solids (VS) added with methane content of 65% whereas fresh and dried pineapple peels gave biogas yields of 0.55% and 0.41 m3/kg VS added and methane content of 51% and 41% respectively.

Ananas↗

PubMed2006

Passive landfill gas emission - Influence of atmospheric pressure and implications for the operation of methane-oxidising biofilters.

A passively vented landfill site in Northern Germany was monitored for gas emission dynamics through high resolution measurements of landfill gas pressure, flow rate and composition as well as atmospheric pressure and temperature. Landfill gas emission could be directly related to atmospheric pressure changes on all scales as induced by the autooscillation of air, diurnal variations and the passage of pressure highs and lows. Gas flux reversed every 20 h on average, with 50% of emission phases lasting only 10h or less. During gas emission phases, methane loads fed to a connected methane oxidising biofiltration unit varied between near zero and 247 g CH4 h(-1)m(-3) filter material. Emission dynamics not only influenced the amount of methane fed to the biofilter but also the establishment of gas composition profiles within the biofilter, thus being of high relevance for biofilter operation. The duration of the gas emission phase emerged as most significant variable for the distribution of landfill gas components within the biofilter.

Air Movements↗

PubMed2001

Denitrification of groundwater with methane as sole hydrogen donor.

It was examined, whether methane can be used as hydrogen donor for an in situ denitrification of groundwater. It is demonstrated, that groundwater can serve as liquid medium and that the denitrification can occur at 10 degrees C. Efforts to enrich methanotrophic bacteria under anoxic conditions have not been successful. No methane oxidation occurred in the absence of oxygen. For this reason, the denitrification with methane must be performed in a two-stage process with aerobic methanotrophic bacteria producing metabolites, that are used as hydrogen donor by non-methanotrophic bacteria in anoxic areas. This kind of indirect denitrification was proved by quantifying nitrogen and nitrous oxide in enrichment cultures that were not stirred or shaken. Large numbers of non-methanotrophic bacteria being able to denitrify with methanol, acetate or proteins as sole hydrogen donor were enriched besides the methanotrophic bacteria under these conditions.

Aerobiosis↗

PubMed2002

Methane yield as a monitoring parameter for the start-up of anaerobic fixed film reactors.

This paper describes the variation of the methane yield during the start-up period of an anaerobic fluidized bed reactor. After a lag phase, with acclimatized sludge, the methane yield increased with time during biofilm development up to the theoretical steady yield value, reported to be around 0.351 CH4/g CODdeg. The establishment of the biofilm required a high consumption of organic material through the microbial synthesis (anabolism), thereby reducing the proportion of substrate converted to methane. As a result, this yield could be an indirect metabolic parameter for evaluating a start-up operation. It could provide vital information about bacterial fixation processes and is easy to be applied to any biofilm reactor, such as anaerobic filters, where biomass sampling is impracticable. Monitoring this parameter could also give useful dynamic information about the different steps of colonization and biomass attachment, which could be used to improve the start-up performance.

Bacteria, Anaerobic↗

PubMed2003

A new gypsum-based technique to reduce methane and phophorus release from sediments of eutrophied lakes: (gypsum treatment to reduce internal loading).

The release of nutrients from the sediment into the water column, i.e. internal nutrient loading, is an important problem in the restoration of eutrophied lakes. The ebullition of gases, mainly methane, has been identified as the key process in nutrient transportation in the internal loading. We studied whether methane production in lake sediment and the release of nutrients into the water column could be prevented by the addition of gypsum (CaSO4 x 2H2O). Three different gypsum products were examined in a controlled laboratory microcosm with a continuous water flow. The addition of gypsum (especially Fe-gypsum) into the sediment increased the redox potentials and reduced methane production and release of phosphorus from the sediments during an incubation period of 3 months. Gypsum evidently acted as a slow-releasing source of sulphate in sediment, which likely enhanced the activity of sulphate-reducing bacteria and improved the overall mineralisation rate of organic matter. The liberation of H2S and phosphate, which might be an undesired consequence of increased sulphate reduction rates was prevented by the application of Fe-containing gypsum likely as a result of the formation of pyrite and apatite minerals.

Calcium Sulfate↗

PubMed2002

Enhanced dehalogenation of halogenated methanes by bimetallic Cu/Al.

A low-cost and high effective copper/aluminum (Cu/Al) bimetal has been developed for treatments of halogenated methanes, including dichloromethane, in near neutral and high pH aqueous systems. Bimetallic Cu/Al was prepared by a simple two-step synthetic method where Cu was deposited onto the Al surface. The presence of Cu on Al significantly enhanced rates of degradation of halogenated methanes and reduced toxic halogenated intermediates. The stability of Cu/Al was preliminarily studied by a multi-spiking batch experiment where complete degradation of carbon tetrachloride was achieved for seven times although the Cu/Al aging was found. Roles of Cu may involve protecting Al against an undesirable oxidation with water, enhancing reaction rates through the galvanic corrosion, and increasing the selectivity to a benign compound (i.e., methane). Kinetic analyses indicated that the activity of bimetallic Cu/Al was comparable to that of iron-based bimetals (e.g., palladized iron) and zero-valent metals. Bimetallic Cu/Al could be a promising reactive reagent for remediation of halogenated solvents-contaminated groundwater associated with high pH problems.

Aluminum↗

PubMed1997

Modification of methane emission in sheep by cysteine and a microbial preparation.

Modification of methane emission from ruminants by the use of L-cysteine and/or a microbial preparation in wethers fed lucerne hay was assessed in an open circuit respiratory trial according to a 4 x 4 Latin squared design. L-Cysteine (0.1 g kg-1 W0.75, as sulphur equivalent) was drenched daily to wethers as an aqueous solution of hydrochloride. The microbial preparation was a dried mixture of Bacillus subtilis, Bacillus cereus, Bacillus thuringiensis, Pseudomonas fluorescens, Streptomyces cellulosae, Streptomyces albidoflavus and Saccharomyces lypolyticum. The microbial preparation was added at 87 mg kg-1 metabolic weight (W0.75) to the daily diet of a wether sheep offered lucerne chaffed hay at a maintenance level of 54 g DM kg-1 W0.75. L-Cysteine suppressed methane emission from the sheep by 13% whereas the microbial preparation actually increased methane emission by 18%. Oxidation-reduction potential, pH, ammonia and VFA were non-significantly influenced by the applied treatments.

Animal Feed↗

PubMed2001

Producing poly-3-hydroxybutyrate with a high molecular mass from methane.

Poly-3-hydroxybutyrate (PHB) and other polyesters can be produced by various species of bacteria. Of the possible carbon sources, methane could provide a suitable substrate for the production of PHB. Methane is cheap and plentiful - not only as natural gas, but also as biogas. The methanotrophic strain Methylocystis sp. GB 25 DSMZ 7674 is able to accumulate PHB in a brief non-sterile process. The studies were carried out using a 7-l and a 70-l pressure bioreactor. Cultivation was performed in two stages: a continuous growth phase (dilution rate 0.17 h(-1)) and a PHB accumulation phase under deficiency conditions of an essential nutrient (ammonium, phosphorus or magnesium) in batch culture. The PHB content of biomass was as high as 51%; efficiency was highest during the first 5 h of the product formation process. The maximum PHB yield relative to the methane consumed was estimated to be 0.55 g g(-1). The PHB produced is of very high quality, having a high molecular mass of up to 2.5x10(6) Da.

Alphaproteobacteria↗

PubMed2001

Methane fluxes from differentially managed grassland study plots: the important role of CH4 oxidation in grassland with a high potential for CH4 production.

Methane oxidation fluxes were monitored with the closed chamber method in eight treatment plots on a semi-wet grassland site near Giessen, Germany. The management regimes differed in the amount of nitrogen (NH4NO3) fertilizer applied and in the height of the in-ground water table. No inhibition of CH4 oxidation occurred, regardless of the amount of annual N fertilizer applied. Instead, the mean CH4 consumption rates were correlated with the mean soil moisture of the plots. However, the correlation between daily soil water content and corresponding CH4 oxidation rate was always weak. During drought period (late summer) water stress was observed to restrict CH4 oxidation rates. The findings led to the question whether methane production with soil depth might modify the CH4 fluxes measured at the surface. Therefore, two new methods were applied: (1) soil air sampling with silicone probes; and (2) anaerobic incubations of soil cores to test for the methane production potential of the grassland soil. The probe measurements revealed that the CH4 sink capacity of a specific site was related to the vertical length of its CH4 oxidizing column, i.e. the depth of the CH4 producing horizon. Anaerobically incubated soil cores produced large amounts of CH4 comparable with tropical rice paddy soil. Under field conditions, heavy autumnal rain in 1998 led to a dramatic increase of soil CH4 concentrations upto 51 microliters l-1 at a depth of 5 cm. Nevertheless, no CH4 was released when soil surface CH4 fluxes were measured simultaneously. The results thus demonstrate the high CH4 oxidation potential of the thin aerobic topsoil horizon in a non-aquatic ecosystem.

Agriculture↗

PubMed2001

Anaerobic biotransformation and methane generation potential of cheese whey in batch and UASB reactors.

Anaerobic treatability and methane generation potential of cheese whey were determined in batch reactors. Furthermore, the effect of nutrient and trace metal supplementation on the batch anaerobic treatment, and the high-rate anaerobic treatability of cheese whey in upflow anaerobic sludge blanket (UASB) reactors were investigated. To this purpose biochemical methane potential experiments were conducted and single- and two-stage UASB reactors with granular cultures were operated. In UASB experiments significance of process staging, operational parameters such as hydraulic retention time (HRT), influent chemical oxygen demand (COD) concentration and loading rate were also investigated. The results revealed that nutrient and trace metal supplementation is vital for the anaerobic treatment of cheese whey; the anaerobic methane generation for the cheese whey studied was found to be 424 ml CH4/g COD (23.4 1 CH4/l cheese whey); undiluted cheese whey could be treated anaerobically at relatively short HRT values (2.06-4.95 days) without any significant stability problems; HRT values as low as 2-3 days can be used for the anaerobic treatment of cheese whey, with a COD removal efficiency of 95-97% at influent COD concentration of 42 700 +/- 141-55 100 +/- 283 mg/l.

Bacteria, Anaerobic↗

PubMed2001

Methane emission factors from cattle manure in Mexico.

Factors responsible for methane emission from cattle manure representing diverse climates, systems and functions of cattle production are presented. These factors were obtained by means of an experimental methodology developed for this project. It was considered that the temperature, moisture, handling of manure and the animals' feed ration affect methane production. Drying conditions and fermentation of manure in cool, temperate and warm climates were simulated in the laboratory. Cattle manure was obtained from animals in intensive, semi-intensive and extensive production systems; for dairy, non-dairy and double purpose cattle production functions. Also handling of manure in dry lot, pasture and solid storage was considered. Results suggest that the dominant factor in methane emissions is the feed ration, followed by fermentation temperature and the excreta moisture content. The emission factors obtained in this work are at least a factor of five smaller than those proposed in the revised 1996 IPCC Guidelines for National Greenhouse Gas Inventories for countries like Mexico.

Animals↗

PubMed2004

Spectroscopic and XRD characterisation of zeolite catalysts active for the oxidative methylation of benzene with methane.

The benzene methylation with methane over zeolite catalysts was previously shown in our laboratory to require the presence of oxygen. Thus, a two-step mechanism involving the intermediate formation of methanol by partial oxidation of methane followed by the methylation of benzene with methanol in the second step, was postulated. This paper now reports the results of the characterisation of the zeolite catalysts used for the oxidative benzene methylation reaction in order to provide some information about their composition, structure, properties and their behaviour before and after the reaction. The catalysts were characterised by X-ray diffraction (XRD), inductively coupled plasma atomic emission spectroscopy (ICP-AES), X-ray fluorescence (XRF), FT-IR and solid state NMR. XRD results indicate that the crystalline structures of all the ZSM-5 and H-beta catalysts remained unchanged after batch reaction of benzene with methane over the catalysts in agreement with the observation that the catalysts recovered from the reactor could be reused without loss of activity. Elemental analyses and FT-IR data show that as the level of metal ion exchange increases, the Brönsted acid concentration decreases but this metal ion exchange does not totally remove Brönsted acidity. FT-IR results further show that only a small amount of acid sites is actually necessary for a catalyst to be active since used catalysts containing highly reduced Brönsted acidity are found to be reusable without any loss of their activity. 29Si and 27Al magic angle spinning (MAS) NMR together with FT-IR spectra also show that all the active zeolites catalysts contain some extra-framework octahedral aluminium in addition to the normal tetrahedral framework aluminium. The presence of this extra-lattice aluminium does not, however, have any adverse effect on the crystallinity of the catalysts both before and after oxidative benzene methylation reaction. There appears also to be no significant dealumination of the zeolite catalysts during reaction since their catalytic performance was retained after use.

Aluminum↗