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PubMed2003

Fluxes of methane, carbon dioxide and nitrous oxide in boreal lakes and potential anthropogenic effects on the aquatic greenhouse gas emissions.

We have examined how some major catchment disturbances may affect the aquatic greenhouse gas fluxes in the boreal zone, using gas flux data from studies made in 1994-1999 in the pelagic regions of seven lakes and two reservoirs in Finland. The highest pelagic seasonal average methane (CH(4)) emissions were up to 12 mmol x m(-2) x d(-1) from eutrophied lakes with agricultural catchments. Nutrient loading increases autochthonous primary production in lakes, promoting oxygen consumption and anaerobic decomposition in the sediments and this can lead to increased CH(4) release from lakes to the atmosphere. The carbon dioxide (CO(2)) fluxes were higher from reservoirs and lakes whose catchment areas were rich in peatlands or managed forests, and from eutrophied lakes in comparison to oligotrophic and mesotrophic sites. However, all these sites were net sources of CO(2) to the atmosphere. The pelagic CH(4) emissions were generally lower than those from the littoral zone. The fluxes of nitrous oxide (N(2)O) were negligible in the pelagic regions, apparently due to low nitrate inputs and/or low nitrification activity. However, the littoral zone, acting as a buffer for leached nitrogen, did release N(2)O. Anthropogenic disturbances of boreal lakes, such as increasing eutrophication, can change the aquatic greenhouse gas balance, but also the gas exchange in the littoral zone should be included in any assessment of the overall effect. It seems that autochthonous and allochthonous carbon sources, which contribute to the CH(4) and CO(2) production in lakes, also have importance in the greenhouse gas emissions from reservoirs.

Atmosphere↗
PubMed2003

Noble metal catalysts for methane removal.

Using a bench-scale rig, the activities of Pt, Pd and Pt+Pd catalysts supported on gamma-Al(2)O(3) and on TiO(2) (anatase) for the complete oxidation of methane (300 ppmv) in air have been measured as a function of temperature; values of T(10), T(50) and T(90) together with the Arrhenius parameters (activation energy and pre-exponential factor) are reported. Pt is less active than Pd when deposited on the surface of the TiO(2), but more active when deposited on gamma-Al(2)O(3), however when combined, the Pt+Pd mixture is more active than either metal individually. The T(10) for Pt+Pd/gamma-Al(2)O(3) was being as low as 228 degrees C. The significance of the Arrhenius parameters, for metal containing catalysts is that they exhibit compensation with increasing activation energy, while securing a more rapid increase in conversion from 0% to 100% when the temperature is increased.

Aluminum Oxide↗
PubMed2000

The long-term evolutions and the regional characteristics of atmospheric methane concentrations in Nagoya, 1983-1997.

This study provides information on the long-term evolutions of the atmospheric methane (CH4) concentrations in Nagoya City, Japan, which were analyzed by using the continuous monitoring data observed at the eight observatory stations for 1983-1997. The 15-year records of the atmospheric CH4 concentrations were examined by means of a time-series analysis using a fast Fourier transform with a low-pass filter to elucidate the seasonal cycles and the long-term trends. The annual averages of the CH4 concentrations in Nagoya were 1.85 ppmv (parts per million by volume), 1.91 ppmv, and 1.90 ppmv in 1988, 1995 and 1997, respectively. Moreover, the annual average growth rate showed a drastic decrease from 17 ppbv (parts per billion by volume) year(-1) in 1992 to 2 ppbv year(-1) in 1993, and further down to 7 ppbv year(-1) in 1997. Comparison of the atmospheric CH4 records in Nagoya with those in global air of the northern hemisphere observed at Mauna Loa observatory in Hawaii, USA, allows us to estimate the excess concentration of CH4 in the urban atmosphere of Nagoya, which was 0.17 ppmv in 1988 and 0.15 ppmv in 1997. On a local scale, the atmospheric CH4 concentrations in the northern part of Nagoya City increased until 1992 and then gradually decreased from 1993 to 1997, although those in the south-western urban areas constantly increased at the averaged growth rate of 13 ppbv year(-1) for 1988-1997. The variation of the long-term trends of the CH4 concentrations in Nagoya may be ascribed to the emission changes from the CH4 sources due to the human activities such as waste dumping and landfills.

Air Pollution↗
PubMed2001

A novel sediment gas sampler and a subsurface gas collector used for measurement of the ebullition of methane and carbon dioxide from a eutrophied lake.

A novel sediment bubble gas sampler and a subsurface bubble gas collector were designed to measure the ebullition of gases from profundal sediments of aquatic ecosystems. The sediment gas sampler was constructed to collect bubble gas samples directly from the uppermost sediment layers for gas composition analysis. The floating subsurface gas collector, designed to trap the bubbles released naturally from sediments, permitted the measurement of both the volume and the composition of the bubble gas. Due to its low cost, light weight and rapid sampling capability, the gas collector is ideal for studies requiring many replicate collectors. These devices were used for measurement of the ebullition of methane (CH4) and carbon dioxide (CO2) during an open water period from hypereutrophic Lake Postilampi, situated within the midboreal zone in Finland. The bubble gas obtained from the sediment with the sediment gas sampler had higher concentrations of CH4 and CO2 than the bubbles trapped in the gas collectors. This indicated that the bubble gas composition changed, either naturally during the migration of the bubbles from the sediment through the water column to the gas collectors, and/or during their storage in the collectors prior to sampling. The mean CH4 ebullition from Lake Postilampi was estimated to be in the range from 36 to 46 mg m(-2 d(-1), based on the bubble gas CH4 concentrations measured from the gas collectors and sediment, respectively. The bubbles contained only 0.02-0.57% of CO2 and thus, the ebullition had no significance in the release of CO2 from the lake.

Carbon Dioxide↗
PubMed1977

Breath-methane in patients with cancer of the large bowel.

In 30 patients with cancer of the large bowel, 24 (80%) had detectable levels of methane in their breath, compared with 25 (39%) of 64 patients with non-malignant large-bowel disease and 83 (40%) of 208 subjects without large-bowel disease. These findings suggest that there may be a difference in anaerobic intestinal flora between patients with cancer of the large bowel and those without the disease. This difference may antedate the development of the tumour or, alternatively, result from the tumour.

Aged↗
PubMed2003

New bis(pyridyl)methane derivatives from 4-hydroxy-2-pyridones: synthesis and antitumoral activity.

Bis(pyridyl)methane derivatives 5-40 were obtained from the reaction of 4-hydroxy-2-pyridones 3 and 4 with aldehydes. Compounds 5-40 were evaluated for cytotoxic activity against a panel of 60 human cancer cell lines by the National Cancer Institute and some of them demonstrated inhibitory effects on the growth of a wide range of cancer cell lines generally at 10(-5) M level and in some case at 10(-7) M concentrations.

Antineoplastic Agents↗
PubMed2002

Gaseous carbon dioxide and methane, as well as dissolved organic carbon losses from a small temperate wetland under a changing climate.

Temperate forests can contain large numbers of wetlands located in areas of low relief and poor drainage. These wetlands can make a large contribution to the dissolved organic carbon (DOC) load of streams and rivers draining the forests, as well as the exchange of methane (CH4) and carbon dioxide (CO2) with the atmosphere. We studied the carbon budget of a small wetland, located in Kejimkujik National Park, Nova Scotia, Canada. The study wetland was the Pine Marten Brook site, a poor fen draining a mixed hardwood-softwood forest. We studied the loss of DOC from the wetland via the outlet stream from 1990 to 1999 and related this to climatic and hydrologic variables. We added the DOC export information to information from a previously published model describing CH4 and CO2 fluxes from the wetland as a function of precipitation and temperature, and generated a new synthesis of the major C losses from the wetland. We show that current annual C losses from this wetland amount to 0.6% of its total C mass. We then predicted that under climate changes caused by a doubling of atmospheric CO2 expected between 2040 and 2050, total C loss from the wetland will almost double to 1.1% of total biomass. This may convert this wetland from what we assume is currently a passive C storage area to an active source of greenhouse gases.

Carbon↗
PubMed2002

Auto-ignition hazard of mixtures of ammonia, hydrogen, methane and air in a urea plant.

The auto-ignition of NH(3)/CH(4)/H(2)/air mixtures constitutes a hazard that is of much concern in urea plants. In this study, the auto-ignition behaviour of NH(3)/CH(4)/H(2)/air mixtures is investigated experimentally for pressures up to 7500 kPa. The experiments were carried out in a closed spherical vessel with a volume of 8 dm(3). The concentration and the pressure dependence of the auto-ignition temperature (AIT) were determined for four types of mixtures: NH(3)/air, NH(3)/CH(4)/air, NH(3)/H(2)/air and NH(3)/CH(4)/H(2)/air. The most ignitable NH(3)/air mixtures were situated between stoichiometry and the upper flammability limit. Small amounts of methane and hydrogen decrease the AIT of NH(3)/air mixtures to a large extent. The pressure dependence of the AIT could be correlated by a Semenov relationship. For the multi-fuel mixtures, a distinct deviation from the Semenov correlation was observed at the lowest temperatures. With respect to the explosion hazard in urea plants, the experimental results were used to assess realistic AIT values in the pool reactor and the ammonia scrubber, operating at a pressure of 15,000 kPa.

Ammonia↗
PubMed2003

The influence of atmospheric pressure on landfill methane emissions.

Landfills are the largest source of anthropogenic methane (CH4) emissions to the atmosphere in the United States. However, few measurements of whole landfill CH4 emissions have been reported. Here, we present the results of a multi-season study of whole landfill CH4 emissions using atmospheric tracer methods at the Nashua, New Hampshire Municipal landfill in the northeastern United States. The measurement data include 12 individual emission tests, each test consisting of 5-8 plume measurements. Measured emissions were negatively correlated with surface atmospheric pressure and ranged from 7.3 to 26.5 m3 CH4 min(-1). A simple regression model of our results was used to calculate an annual emission rate of 8.4 x 10(6) m3 CH4 year(-1). These data, along with CH4 oxidation estimates based on emitted landfill gas isotopic characteristics and gas collection data, were used to estimate annual CH4 generation at this landfill. A reported gas collection rate of 7.1 x 10(6) m3 CH4 year(-1) and an estimated annual rate of CH4 oxidation by cover soils of 1.2 x 10(6) m3 CH4 year(-1) resulted in a calculated annual CH4 generation rate of 16.7 x 10(6) m3 CH4 year(-1). These results underscore the necessity of understanding a landfill's dynamic environment before assessing long-term emissions potential.

Atmospheric Pressure↗
PubMed2000

Regulation of expression of methane monooxygenases by copper ions.

Many methanotrophs contain both a soluble and a particulate methane monooxygenase. A unique metabolic switch, mediated by copper ions, regulates the expression of these enzymes. When the copper-to-biomass ratio of the cell is low, the soluble enzyme is expressed, and when the copper-to-biomass ratio is high, the particulate enzyme is expressed. A model for the mechanism of this switch is proposed.

Base Sequence↗
PubMed2002

Can methane suppression during digestion of woody and leafy browse compensate for energy costs of detoxification of plant secondary compounds? A test with muskoxen fed willows and birch.

Digestion and metabolism of woody and leafy browse requires detoxification of plant secondary compounds that can incur an energy cost. Browse, however, inhibits methane (CH(4)) production and therefore could offset some costs of detoxification. We measured an index of heat increment of feeding (HIFi) and CH(4) production in muskoxen (Ovibos moschatus) given a single test meal (at 10 g/kg BM(0.75)) composed of hay mixed with one of three browse species (Willow: Salix alaxensis, S. pulchra; Birch: Betula nana). Detoxification cost was estimated as HIFi of browse diet-HIFi of hay diet and CH(4) compensation as CH(4) production of hay diet-CH(4) production of browse diet. CH(4) compensation was noted in 47% of 15 trials in which a detoxification cost was evident; six trials were with woody browse and one with leafy browse. Separate controls were responsible for the difference in CH(4) compensation for leafy browse vs. woody browse. Detoxification costs for twigs and leaves of B. nana were underestimated because of their low digestibility. In only one of six treatments was CH(4) compensation documented for B. nana. We conclude that energy saved by CH(4) suppression was small (<6%) compared with detoxification costs.

Animal Feed↗
PubMed2002

Towards accurate ab initio predictions of the vibrational spectrum of methane.

We have carried out extensive ab initio calculations of the electronic structure of methane, and these results are used to compute vibrational energy levels. We include basis set extrapolations, core-valence correlation, relativistic effects, and Born-Oppenheimer breakdown terms in our calculations. Our ab initio predictions of the lowest lying levels are superb.

Chemical Phenomena↗
PubMed2002

A perturbative calculation of the rovibrational energy levels of methane.

The rovibrational energy levels of methane are determined from a quartic ab initio potential energy force field where the expansion coordinates are the Morse coordinates for the stretches and extension coordinates for the bends. Energies are calculated using canonical Van Vleck perturbation theory. Results are obtained for both rotation-vibration Hamiltonians expressed as functions of curvilinear and rectilinear normal coordinates. Second, fourth, and sixth order curvilinear results are compared with experimental results, and fourth order results for the rectilinear and curvilinear Hamiltonian are compared to each other. The calculated rovibrational levels are in good agreement with the experimental values for low J levels. The calculated rotational level splittings are in even better agreement with the experiment. In particular, the ground state tetrahedral splittings, which are as small as 10(-4) cm(-1), are well reproduced by our calculations at sixth order.

Chemical Phenomena↗
PubMed2002

High-precision isotopic ratio measurement system for methane (12CH3D/12CH4,13CH4/12CH4) by using near-infrared diode laser absorption spectroscopy.

We demonstrate that the absorption spectroscopic method can be applied to a precise deltaD (an index of 12CH3D/12CH4) and delta13C (an index of 13CH4/12CH4) analysis for methane samples of natural isotopic abundance. We chose an appropriate absorption line pair whose absorption coefficients have nearly the same temperature dependences so as to minimize the temperature effect in absorbance ratio measurements. We measured 12CH3D/12CH4 ratio by using near-infrared external cavity diode lasers and a new type multi-pass cell. The deltaD value can be determined from the 12CH3D/12CH4 signal-intensity ratio with a fine correction by taking account of the interference of 13CH4 lines. Similarly, the delta13C value is determined from the 13CH4/12CH4 signal-intensity ratio, which is measured by using distributed-feedback laser and a modified Herriot-type cell and corrected for the abundance of 12CH3D. The precision was +/-0.7 and +/-0.027/1000 for deltaD and delta13C, respectively.

Carbon Isotopes↗
PubMed1985

Methanofuran (carbon dioxide reduction factor), a formyl carrier in methane production from carbon dioxide in Methanobacterium.

Methanofuran (carbon dioxide reduction factor) became labeled when incubated in cell extracts of Methanobacterium under hydrogen and 14CO2 in the absence of methanopterin. Proton NMR spectroscopy revealed that a formyl group was bound to the primary amine of methanofuran. [14C]Formylmethanofuran was enzymically converted to 14CH4 in the presence of CH3-S-CoM [2-(methylthio)ethanesulfonic acid], hydrogen, and methanopterin, establishing the formyl moiety as an intermediate in methanogenesis. In the absence of methanopterin, a substantial portion of the formyl label was oxidized to 14CO2 rather than reduced to 14CH4, consistent with a model in which the C1 intermediate is first bound to methanofuran and then to methanopterin, during its reduction. When CH3-S-CoM was replaced by HS-CoM (2-mercaptoethanesulfonic acid), most of the formyl label was oxidized to 14CO2, indicating that methyl group reduction by the CH3-S-CoM methylreductase is required for the conversion of formylmethanofuran to methane.

Carbon Dioxide↗
PubMed1997

Roles of the methane monooxygenase reductase component in the regulation of catalysis.

The reductase component (MMOR) of the soluble methane monooxygenase isolated from Methylosinus trichosporium OB3b catalyzes transfer of 2e- from NADH to the hydroxylase component (MMOH) where oxygen activation and substrate oxidation occur. It is shown here that MMOR can also exert regulatory effects on catalysis by binding to MMOH or to the binary complex of MMOH and component B (MMOB), another regulatory protein. MMOR alters the oxidation-reduction potentials of the dinuclear iron cluster at the active site of MMOH. Although little change is observed in the potential for the first electron transfer to the cluster (E(1)0' = 76 mV), the E(2)0' potential value for the second electron transfer is increased from 21 to 125 mV. This shift provides a larger driving force for electron transfer from MMOR and favors transfer of two rather than one electron as required by catalysis. Similar positive shifts in potential are observed even in the presence of MMOB which has been shown to cause a 132 mV negative shift in the midpoint potential of MMOH in the absence of MMOR. MMOR is also shown to decrease the rate of reaction between the fully reduced MMOH-MMOB and O2 approximately 20-fold at 4 degrees C. However, the time course of the key catalytic cycle intermediate that can react with substates, compound Q, is unaffected. This implies a compensating faster decay of one or more of the intermediates that occur between diferrous MMOH and compound Q in the reaction cycle, thereby limiting potential nonproductive autodecay of these intermediates. Accordingly, an increase in single turnover product yield is observed in the presence of MMOR. Interestingly, MMOR can cause the redox potential increases, changes in rates, and the increase in product yield when present at only 10% of the concentration of MMOH active sites. Substrate binding is shown to induce negligible changes in the redox potentials. Two alternative regulatory schemes are presented based on (i) thermodynamic coupling of component binding and redox changes or (ii) dynamic interconversion of two states of MMOH promoted by MMOR.

Catalysis↗
PubMed2002

Reduction of polyhalogenated methanes by surface-bound Fe(II) in aqueous suspensions of iron oxides.

Uptake of ferrous iron from aqueous solution by iron oxides results in the formation of a variety of reactive surface species capable of reducing polyhalogenated methanes (PHMs). Pseudo-first-order reaction rate constants, k(obs), of PHMs increased in the order CHBrCl2 < CHBr2Cl < CHBr3 < CCl4 < CFBr3 < CBrCl3 < CBr2Cl2. The k(obs) values increased with the exposure time, teq, of Fe(II) to suspended iron oxides which was attributed to the rearrangement of initially sorbed Fe(II) species to more reactive surface species with time. At pH 7.2, the k(obs) values of PHMs also increased with the concentration of surface-bound ferrous iron, Fe(II)sorb, particularly when Fe(II)tot was increased to concentrations where surface precipitation becomes likely. At fixed total Fe(II) concentrations, k(obs) values increased exponentially with pH. The highest reactivities were associated with pH conditions where surface precipitation of Fe(II) is expected. Fe(II)sorb and pH, however, had opposite effects on the product formation of PHMs. At pH 7.2, the formation of formate from CX4 (X = CI, Br) increased with Fe(II)sorb, whereas increasing pH favored the formation of CHX3. The ratio of halogenated products and formate formed is indicative of the relative importance of initial one- or two-electron-transfer processes, respectively, and was found to depend on the type of iron oxide mineral also. Our data form a basis to assess the importance of chemical reactions in natural attenuation processes of PHMs in environmental systems under iron-reducing conditions.

Ferric Compounds↗
PubMed2002

Syntheses and solid state structures of tris(pyrazolyl)methane complexes of sodium, potassium, calcium, and strontium: comparison of structures with analogous complexes of lead(II).

The reaction of NaI with 2 equiv of HC(pz)(3) or HC(3,5-Me(2)pz)(3) (pz = pyrazolyl ring) leads to the formation of [[HC(pz)(3)](2)Na](I) (1) and [[HC(3,5-Me(2)pz)(3)](2)Na](I) (2), respectively. Both compounds have trigonally distorted octahedral arrangements about the sodium. A similar reaction of KPF(6) with HC(3,5-Me(2)pz)(3) results in the formation of [[HC(3,5-Me(2)pz)(3)](2)K](PF(6)) (3), a complex also shown crystallographically to have a trigonally distorted octahedral arrangement about the potassium, which is an unusually low coordination number for this large metal ion. The complex [[HC(pz)(3)](2)Sr](BF(4))(2) (4) forms in the reaction of Sr(acac)(2) (acac = acetylacetonate) with HBF(4).Et(2)O followed by 2 equiv of HC(pz)(3). The structure is highly distorted, showing kappa(3) bonding of both tris(pyrazolyl)methane ligands and, in addition, interactions with the metal from three fluorine atoms from the BF(4)(-) counterions. The symmetrical structure of 1 and the nine-coordinate structure of 4 are both very different from the distorted, six-coordinate structure [[HC(pz)(3)](2)Pb](BF(4))(2), indicating that for this compound the lone pair on lead(II) is influencing the structure. The reaction of M(acac)(2) (M = Sr, Ca) with H[B[3,5-(CF(3))(2)C(6)H(3)](4)] followed by 2 equiv of HC(pz)(3) produces [[HC(pz)(3)](2)(Hacac)Sr][B[3,5-(CF(3))(2)C(6)H(3)](4)](2) (5) (when the reaction is done in CH(2)Cl(2)), [[HC(pz)(3)](2)(Me(2)CO)(2)Sr][B[3,5-(CF(3))(2)C(6)H(3)](4)](2) (6) (when the reaction is done in acetone), and [[HC(pz)(3)](2)(Hacac)Ca][B[3,5-(CF(3))(2)C(6)H(3)](4)](2)(7), respectively. The structures of all three complexes show a distorted eight-coordinate arrangement of the ligands about the metal. Crystal data: 1 is orthorhombic, Pnma, a = 16.931(1), b = 22.368(3), c = 7.937(2) A, alpha = 90, beta = 90, gamma = 90 degrees, Z = 4; 2 is trigonal, R3, a = 10.7483(8), b = 10.7483(8), c = 35.395(4) A, alpha = 90, beta = 90, gamma = 120 degrees, Z = 3; 3 is monoclinic, P2(1)/c, a = 9.144(4), b = 13.377(6), c = 15.988(7) A, alpha = 90, beta = 92.291(10), gamma = 90 degrees, Z = 2; 4 is hexagonal, P6(5), a = 9.42530(10), b = 9.42530(10), c = 55.3713(5) A, alpha = 90, beta = 90, gamma = 120 degrees, Z = 6; 5 is monoclinic, P2/n, a = 14.1601(3), b = 13.1756(3), c = 27.1826(6) A, alpha = 90, beta = 90.1744(7), gamma = 90 degrees, Z = 2; 6 is monoclinic, P2/n, a = 14.2709(7), b = 13.2646(7), c = 27.4189(13) A, alpha = 90, beta = 90.3850(10), gamma = 90 degrees, Z = 2; 7 is monoclinic, P2/n, a = 14.2388(2), b = 13.1919(2), c = 26.7879(3) A, alpha = 90, beta = 90.0650(8), gamma = 90 degrees, Z = 2.

Algorithms↗