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PubMed2004

Methane oxidation and formation of EPS in compost: effect of oxygen concentration.

Oxygen concentration plays an important role in the regulation of methane oxidation and the microbial ecology of methanotrophs. However, this effect is still poorly quantified in soil and compost ecosystems. The effect of oxygen on the formation of exopolymeric substances (EPS) is as yet unknown. We studied the effect of oxygen on the evolution of methanotrophic activity. At both high and low oxygen concentrations, peak activity was observed twice within a period of 6 months. Phospholipid fatty acid analysis showed that there was a shift from type I to type II methanotrophs during this period. At high oxygen concentration, EPS production was about 250% of the amount at low oxygen concentration. It is hypothesized that EPS serves as a carbon cycling mechanism for type I methanotrophs when inorganic nitrogen is limiting. Simultaneously, EPS stimulates nitrogenase activity in type II methanotrophs by creating oxygen-depleted zones. The kinetic results were incorporated in a simulation model for gas transport and methane oxidation in a passively aerated biofilter. Comparison between the model and experimental data showed that, besides acting as a micro-scale diffusion barrier, EPS can act as a barrier to macro-scale diffusion, reducing the performance of such biofilters.

Animals↗
PubMed2006

Long-term aerobic cometabolism of a chlorinated solvent mixture by vinyl chloride-, methane- and propane-utilizing biomasses.

The aerobic cometabolic biodegradation of a mixture of chlorinated aliphatic hydrocarbons (CAHs) including vinyl chloride (VC), cis- and trans-1,2-dichloroethylene (cis-DCE, trans-DCE), trichloroethylene (TCE), 1,1,2-trichloroethane (1,1,2-TCA) and 1,1,2,2-tetrachloroethane (1,1,2,2-TeCA) was investigated at both 25 and 17 degrees C by means of bioaugmented and non-bioaugmented sediment-groundwater slurry microcosm tests. The goals of the study were (i) to study the long-term aerobic biodegradation of a CAH mixture including a high-chlorinated solvent (1,1,2,2-TeCA) generally considered non-biodegradable in aerobic conditions; (ii) to investigate the efficacy of bioaugmentation with two types of internal inocula obtained from the indigenous biomass of the studied site; (iii) to identify the CAH-degrading bacteria. VC, methane and propane were utilized as growth substrates. The non-bioaugmented microcosms were characterized, at 25 degrees C, by an average 18-day lag-time for the direct metabolism of VC (accompanied by the cometabolism of cis- and trans-DCE) and by long lag-times (36-264 days) for the onset of methane or propane utilization (associated with the cometabolism of the remaining CAHs). In the inoculated microcosms the lag-phases for the onset of growth substrate utilization and CAH cometabolism were significantly shorter (0-15 days at 25 degrees C). Biodegradation of the 6-CAH mixture was successfully continued for up to 410 days. The low-chlorinated solvents were characterized by higher depletion rates. The composition of the microbial consortium of a propane-utilizing microcosm was determined by 16s rDNA sequencing and phylotype analysis. To the best of our knowledge, this is the first study that documents the long-term aerobic biodegradation of 1,1,2,2-TeCA.

Aerobiosis↗
PubMed2004

Butachlor inhibits production and oxidation of methane in tropical rice soils under flooded condition.

In laboratory incubation experiments, application of a commercial formulation of the herbicide butachlor (N-butoxymethyl-2-chloro-2',6'-diethyl acetanilide) to three tropical rice soils, widely differing in their physicochemical characteristics, under flooded condition inhibited methane (CH4) production. The inhibitory effect was concentration dependent and most remarkable in the alluvial soil. Thus, following application of butachlor at 5, 10, 50 and 100 microg g(-1) soil, respectively, cumulative CH4 production in the alluvial soil was inhibited by 15%, 31%, 91% and 98% over unamended control. Since CH4 production was less pronounced in the sandy loam and acid sulfate soil, the impact of amendment with butchalor, albeit inhibitory, was less extensive than the alluvial soil. Inhibition of CH4 production in butachlor-amended alluvial soil was related to the prevention in the drop in redox potential as well as low methanogenic bacterial population especially at high concentrations of butachlor. CH4 oxidation was also inhibited in butachlor-amended alluvial soil with the inhibitory effect being more prevalent under flooded condition. Inhibition in CH4 oxidation was related to a reduction in the population of soluble methane monooxygenase producing methanotrophs. Results demonstrate that butachlor, a commonly used herbicide in rice cultivation, even at very low concentrations can affect CH4 production and its oxidation, thereby influencing the biogeochemical cycle of CH4 in flooded rice soils.

Acetanilides↗
PubMed2006

Two-channel opto-acoustic diode laser spectrometer and fine structure of methane absorption spectra in 6070-6180 cm-1 region.

We describe the hardware and software of the high-sensitive two-channel opto-acoustic spectrometer with a near infrared diode laser. A semiconductor TEC-100 laser with outer resonator generates a continuous single-frequency radiation in the range of 6040-6300 cm-1 with spectral resolution better that 10 MHz. The newly designed model of photo-acoustic cells in the form of a ring type resonator was used in the spectrometer, and the system allows the measurement of a weak absorption coefficient equal to 1.4x10(-7) cm-1 Hz-1/2 with a laser radiation power of 0.003 W. The methane absorption spectra within a range of 6080-6180 cm-1 were measured with a spectral resolution of 10 MHz and the signal to noise ratio more than 10(3). Six hundred absorption lines were recorded, which is twice as many as in HITRAN-2004. The accurate measurements of the half-width and shift of methane unresolved triplet R3 of 2nu3 band permit us to determine values of the broadening and shift coefficients for CH4-air, CH4-N2, and CH4-SF6 mixtures.

Acoustics↗
PubMed2004

Methane emissions from a constructed wetland treating wastewater--seasonal and spatial distribution and dependence on edaphic factors.

Constructed wetlands for wastewater treatment have many advantages. They can be used for several purposes, for example, to reduce levels of organic matter and nutrients, and to retain toxic metals. However, most wetlands are inherently net sources of gaseous compounds like methane and nitrous oxide, which are of environmental concern due to their rapid current accumulation in the atmosphere and their potent global warming capacity. In order to determine the flux of methane from a constructed wetland a study was conducted over two growth seasons on a pilot scale wetland constructed to reduce nutrient levels in secondary treated wastewater. The emissions for the spring to autumn period averaged 141 mg CH(4)m(-2)d(-1) (S.D.=187), ranging from consumption of 375 mg CH(4)m(-2)d(-1) to emissions of 1739 mg CH(4)m(-2)d(-1). The spatial and temporal variations were large, but could be accounted for by measured environmental factors. Among these factors, sediment and water temperatures were significant in all cases and independent of the scale of analysis (r(2) up to 0.88).

Ecosystem↗
PubMed2003

Determination of carbon monoxide, methane and carbon dioxide in refinery hydrogen gases and air by gas chromatography.

This paper illustrates a method for determining trace amounts of CO, CH4 and CO2 with the detection limit of 0.15, 0.15 and 0.20 microg/l, respectively, in refinery hydrogen gases or in air. A simple modification of a gas chromatograph equipped with a flame-ionization detector is presented. A Porapak Q column, additionally connected with a short molecular sieve 5A packed column and a catalytic hydrogenation reactor on the Ni catalyst have been applied. The principle of the analytical method proposed is the separation of CO from O2 before the introduction of CO to the methanizer. The analytical procedure and examples of the results obtained have been presented. The modification applied makes it possible to use the GC instrument for other determinations, requiring utilization of the Porapak Q column and the flame-ionization detector. In such cases, the short molecular sieve 5A column and the methanizer can be by-passed.

Carbon Dioxide↗
PubMed2003

Chemistry of trace elements in coalbed methane product water.

Extraction of methane (natural gas) from coal deposits is facilitated by pumping of aquifer water. Coalbed methane (CBM) product water, produced from pumping ground water, is discharged into associated unlined holding ponds. The objective of this study was to examine the chemistry of trace elements in CBM product water at discharge points and in associated holding ponds across the Powder River Basin, Wyoming. Product water samples from discharge points and associated holding ponds were collected from the Cheyenne River (CHR), Belle Fourche River (BFR), and Little Powder River (LPR) watersheds during the summers of 1999 and 2000. Samples were analyzed for pH, Al (aluminum), As (arsenic), B (boron), Ba (barium), Cr (chromium), Cu (copper), F (fluoride), Fe (iron), Mn (manganese), Mo (molybdenum), Se (selenium), and Zn (zinc). Chemistry of trace element concentrations were modeled with the MINTEQA2 geochemical equilibrium model. Results of this study show that pH of product water for three watersheds increased in holding ponds. For example the pH of CBM product water increased from 7.21 to 8.26 for LPR watershed. Among three watersheds, the CBM product water exhibited relatively less change in trace element concentrations in CHR watershed holding ponds. Concentration of dissolved Al, Fe, As, Se, and F in product water increased in BFR watershed holding ponds. For example, concentration of dissolved Fe increased from 113 to 135 microg/L. Boron, Cu, and Zn concentrations of product water did not change in BFR watershed holding ponds. However, concentration of dissolved Ba, Mn, and Cr in product water decreased in BFR watershed holding ponds. For instance, Ba and Cr concentrations decreased from 445 to 386 microg/L and from 43.6 to 25.1 microg/L, respectively. In the LPR watershed, Al, Fe, As, Se, and F concentrations of product water increased substantially in holding ponds. For example, Fe concentration increased from 192 to 312 microg/L. However, concentration of dissolved Ba, Mn, Cr, and Zn decreased in holding ponds. Geochemical modeling calculations suggested that observed increase of Al and Fe concentrations in holding ponds was due to increase in concentration of Al(OH)(4)(-) and Fe(OH)(4)(-) species in water which were responsible for pH increases. Decreases in Ba, Mn, Cr, and Zn concentrations were attributed to the increase in pH, resulting in precipitates of BaSO(4) (barite), MnCO(3) (rhodochrosite), Cr(OH)(2) (chromium hydroxide), and ZnCO(3) (smithsonite) in pond waters, respectively.

Coal Mining↗
PubMed2003

Selective optimization in thermophilic acidogenesis of cheese-whey wastewater to acetic and butyric acids: partial acidification and methanation.

For partial acidogenesis of cheese-whey wastewater, a set of experiments were carried out to produce short-chain volatile fatty acids (VFA) in laboratory-scale continuously stirred tank reactors (CSTR). The maximum rate of acetic and butyric acid production associated with simultaneous changes in hydraulic retention time (HRT), pH, and temperature was investigated, in which the degree of acidification of the whey to the short-chain VFAs was less than 20% of the influent chemical oxygen demand (COD) concentration. Response surface methodology was successfully applied to determine the optimum physiological conditions where the maximum rates of acetic and butyric acid production occurred. These were 0.40-day HRT, pH 6.0 at 54.1 degrees C and 0.22-day HRT, pH 6.5 at 51.9 degrees C, respectively. The optimum conditions for acetic acid production were selected for partial acidification of cheese-whey wastewater because of a higher rate in combined productions of acetic and butyric acids than that at optimum conditions for butyric acid production. A thermophilic two-phase process with the partial acidification followed by a methanation step was operated. Performance of the two-phase process was compared to the single-phase anaerobic system. The two-phase process clearly showed a better performance in management of cheese-whey wastewater over the single-phase system. Maximum rate of COD removal and the rate of methane production in the two-phase process were, respectively, 116% and 43% higher than those of the single-phase system.

Bacteria, Anaerobic↗
PubMed2002

Ozone effects on Sphagnum mosses, carbon dioxide exchange and methane emission in boreal peatland microcosms.

Microcosms of a boreal peatland originating from an oligotrophic fen in Eastern Finland were fumigated under four ozone concentrations (0, 50, 100 and 150 ppb O3) in laboratory growth chambers during two separate experiments (autumn and summer) for 4 and 6 weeks, respectively. Ozone effects on Sphagnum mosses and the fluxes of carbon dioxide and methane were evaluated. In both experiments, the three Sphagnum species studied showed only a few significant responses to ozone. In the autumn experiment, membrane permeability of S. angustifolium, measured as conductivity and magnesium leakage, was significantly higher under ozone fumigation (P = 0.005 and < 0.001, respectively), and there was a distinct dose-dependence. S. magellanicum showed no clear responses, either for membrane leakage or pigment content. There were no substantial ozone responses in the gross photosynthesis or net CO2 exchange during the 6-week-long summer experiment, but dark ecosystem respiration was transiently increased by ozone concentration of 100 ppb after 14 days of exposure (P < 0.05). Fumigation with 100 ppb of ozone, however, more than doubled (P < 0.05) methane emission from the peatland monoliths. Our results suggest that increasing tropospheric ozone concentration may cause substantial changes in the carbon gas cycling of boreal peatlands, even though these changes are not closely associated with the changes in Sphagnum vegetation.

Bryopsida↗
PubMed2001

Exploring correlation between redox potential and other edaphic factors in field and laboratory conditions in relation to methane efflux.

Methane is primarily a biogenic gas, which is implicated in global warming. Although its production in the anoxic conditions is regulated by several edaphic factors, aquatic macrophytes also influence methane emission by providing aerenchyma to act as chimney for CH4 transport from the sediment to troposphere, by releasing root exudates to the sediment to serve as substrate for methanogenic bacteria and by transporting atmospheric O2 to rhizosphere, which stimulates CH4 consumption. Among the edaphic factors, redox potential (Eh) is the most important, which largely determines the action of methanogenic bacteria. Hence, a study was undertaken first to find out the correlation between CH4 emission and edaphic factors in the field conditions and then to understand the relationship between Eh and other edaphic factors. The field studies revealed that natural wetlands were the major source of CH4 emission, and the vegetation plays an important role in CH4 emission from the water bodies. However, it was very difficult to establish a strong relationship between the CH4 emission and the edaphic factors in the field conditions due to other limiting factors and their constant fluctuations. In this connection, the laboratory experiments exhibited that soil temperature, pH, moisture regime and incubation period were negatively correlated with Eh, which determines the initiation of methanogenic process. However, organic carbon and the water regime over the soil surface did not show any impact on Eh in this study.

Air Pollutants↗
PubMed2002

Gold helps bacteria to oxidize methane.

With the use of labeled methane-14C and by chromatographic analysis it was shown that gold-containing protein ("Au-protein"), isolated from goldphilic Micrococcus luteus bacteria, catalyzes the oxidation of methane to methanol in the system also containing NADH, air, K(3)Fe(CN)(6) and Tris-HCl buffer. Presumably Au-protein helps bacteria to survive when usual sources of carbon and energy are scarce.

Gold↗
PubMed1990

Catalysis of carbon monoxide methanation by deep sea manganate minerals.

The catalytic activity of deep sea manganese nodule minerals for the methanation of carbon monoxide was measured with a microcatalytic technique between 200 and 460 degrees C. The manganate minerals were activated at 248 degrees C by immersion into a stream of hydrogen in which pulses of carbon monoxide were injected. Activation energies for the methanation reaction and hydrogen desorption from the manganate minerals were obtained and compared with those of pure nickel. Similar energy values indicate that the activity of the nodule materials for the reaction appears to be related to the amount of reducible transition metals present in the samples (ca. 11 wt.-%). Since the activity of the nodule minerals per gram is comparable to that of pure nickel, most of the transition metal ions located between manganese oxide layers appear to be exposed and available to catalyze the reaction.

Carbon Monoxide↗
PubMed2001

Oxidation of activated carbon and methane using a high-frequency pulsed plasma.

We have demonstrated a new method using a high-frequency pulsed plasma for oxidizing methane and activated carbon powder (1-150 microm) as two substitutes for diesel particulate matter (PM). Methane and activated carbon can be oxidized at a rate of 4-40 and 4-10g-CH(4)/kWh, respectively. A discussion on future development of this technology is given.

Air Pollution↗
PubMed2000

Spin glass formation in La0.9Sr0.1CoO3 catalyst for flameless combustion of methane.

Two samples of composition La0.9M0.1CoO3 (M = Sr, Ce) have been compared as catalysts for the flameless combustion of methane. The former showed a lower activity than the latter and this difference was enhanced at lower temperature. Aiming at understanding the origin of this behaviour, EPR analysis was carried out at temperatures down to 100 K. At T < 245 K a zero-field intense feature appeared with the M = Sr sample only, characterized by opposite phase with respect to the g approximately 2 line. This zero-field line was attributed to microwave absorption by spin glass formed by cobalt- and oxygen-based paramagnetic ions. The tendency to strong interaction among these species could also be a reason of the low oxygen availability for the catalytic methane oxidation at higher temperature.

Catalysis↗
PubMed1975

New inhibitors of methane production by rumen micro-organisms. Development and testing of inhibitors in vitro.

1. A procedure is described for assaying in vitro the activity of various inhibitors of methane production by rumen micro-organisms. 2. Methods of preparation of various inhibitors are described together with attempts to characterize these compounds by determining their physical properties (physical state, density, chromatographic behaviour), their hydrolysis by rumen contents and their relative potency as inhibitors. 3. The results of preliminary studies with trichloroethanol and its ester with pivalic acid are given. 4. The inhibitory activities of several groups of related compounds are reported. These include the polyhalogenated alcohols and their esters with pivalic acid, the esters of trihalogenated alcohols and monobasic fatty acids from C2 and C16 and the trihalogenated alcohol esters of dibasic acids. The results of experiments with esters of alcohols and polyhalogenated carboxylic and sulphonic acids are also given. 5. It is concluded that the mechanism of action of the inhibitors might be similar to that of known polyhalogenated methane analogues (e.g. chloroform). The relative activity of various compounds might be partly governed by the ease of their absorption into the microbial cells and by the extent to which the esters can be hydrolysed by rumen contents. 6. The results show that some substances are very poor inhibitors, unless they are esterified (e.g. trichloroacetic acid) but on the whole the esters in which the polyhalogen grouping is on the alcohol portion of the molecule are better inhibitors than those in which it is on the acid portion of the molecule.

Animals↗
PubMed2003

Scientific basis for process and catalyst design in the selective oxidation of methane to formaldehyde.

The mechanism and kinetics of the gas-phase selective oxidation of methane to formaldehyde (MPO) are revised in the general context of catalytic oxidations. In agreement with ab initio calculations of the energy barrier for the activation of methane on transition metal oxide complexes, a formal Langmuir-Hinshelwood kinetic model is proposed which accounts for the "steady-state" conditions and activity-selectivity pattern of MPO catalysts, providing an original support to process design and catalyst development.

Catalysis↗
PubMed2006

Role of the C-terminal region of the B component of Methylosinus trichosporium OB3b methane monooxygenase in the regulation of oxygen activation.

The effects of the C-terminal region of the B component (MMOB) of soluble methane monooxygenase (sMMO) from Methylosinus trichosporium OB3b on steady-state turnover, the transient kinetics of the reaction cycle, and the properties of the sMMO hydroxylase (MMOH) active site diiron cluster have been explored. MMOB is known to have many profound effects on the rate and specificity of sMMO. Past studies have revealed specific roles for the well-folded core structure of MMOB as well as the disordered N-terminal region. Here, it is shown that the disordered C-terminal region of MMOB also performs critical roles in the regulation of catalysis. Deletion mutants of MMOB missing 5, 8, and 13 C-terminal residues cause progressive decreases in the maximum steady-state turnover number, as well as lower apparent rate constants for formation of the key reaction cycle intermediate, compound Q. It is shown that this latter effect is actually due to a decrease in the rate constant for formation of an earlier intermediate, probably the hydroperoxo species, compound P. Moreover, the deletions result in substantial uncoupling at or before the P intermediate. It is proposed that this is due to competition between slow H(2)O(2) release from one of the intermediates and the reaction that carries this intermediate on to the next step in the cycle, which is slowed by the mutation. Electron paramagnetic resonance (EPR) studies of the hydroxylase component (MMOH) in the mixed valent state suggest that complexation with the mutant MMOBs alters the electronic properties of the diiron cluster in a manner distinct from that observed when wild-type MMOB is used. Active site structural changes are also suggested by a substantial decrease in the deuterium kinetic isotope effect for the reaction of Q with methane thought to be associated with a decrease in quantum tunneling in the C-H bond breaking reaction. Thus, the surface interactions between MMOH and MMOB that affect substrate oxidation and its regulation appear to require the complete MMOB C-terminal region for proper function.

Amino Acid Sequence↗
PubMed1999

Component interactions in the soluble methane monooxygenase system from Methylococcus capsulatus (Bath).

The soluble methane monooxygenase system of Methylococcus capsulatus (Bath) includes three protein components: a 251-kDa non-heme dinuclear iron hydroxylase (MMOH), a 39-kDa iron-sulfur- and FAD-containing reductase (MMOR), and a 16-kDa regulatory protein (MMOB). The thermodynamic stability and kinetics of formation of complexes between oxidized MMOH and MMOB or MMOR were measured by isothermal titration calorimetry and stopped-flow fluorescence spectroscopy at temperatures ranging from 3.3 to 45 degrees C. The results, in conjunction with data from equilibrium analytical ultracentrifugation studies of MMOR and MMOB, indicate that free MMOR and MMOB exist as monomers in solution and bind MMOH with 2:1 stoichiometry. The role of component interactions in the catalytic mechanism of sMMO was investigated through simultaneous measurement of oxidase and hydroxylase activities as a function of varied protein component concentrations during steady-state turnover. The partitioning of oxidase and hydroxylase activities of sMMO is highly dependent on both the MMOR concentration and the nature of the organic substrate. In particular, NADH oxidation is significantly uncoupled from methane hydroxylation at MMOR concentrations exceeding 20% of the hydroxylase concentration but remains tightly coupled to propylene epoxidation at MMOR concentrations ranging up to the MMOH concentration. The steady-state kinetic data were fit to numerical simulations of models that include both the oxidase activities of free MMOR and of MMOH/MMOR complexes and the hydroxylase activity of MMOH/MMOB complexes. The data were well described by a model in which MMOR and MMOB bind noncompetitively at distinct interacting sites on the hydroxylase. MMOB manifests its regulatory effects by differentially accelerating intermolecular electron transfer from MMOR to MMOH containing bound substrate and product in a manner consistent with its activating and inhibitory effects on the hydroxylase.

Catalysis↗