Plume mapping and isotopic characterisation of anthropogenic methane sources

Methane stable isotope analysis, coupled with mole fraction measurement, has been used to link isotopic signature to methane emissions from landfill sites, coal mines and gas leaks in the United Kingdom. A mobile Picarro G2301 CRDS (Cavity Ring-Down Spectroscopy) analyser was installed on a vehicle, together with an anemometer and GPS receiver, to measure atmospheric methane mole fractions and their relative location while driving at speeds up to 80 kph. In targeted areas, when the methane plume was intercepted, air samples were collected in Tedlar bags, for delta C-13-CH4 isotopic analysis by CF-GC-IRMS (Continuous Flow Gas Chromatography-Isotope Ratio Mass Spectrometry). This method provides high precision isotopic values, determining delta C-13-CH4 to +/- 0.05 per mil. The bulk signature of the methane plume into the atmosphere from the whole source area was obtained by Keeling plot analysis, and a delta C-13 -CH4 signature, with the relative uncertainty, allocated to each methane source investigated. Both landfill and natural gas emissions in SE England have tightly constrained isotopic signatures. The averaged delta C-13-CH4 for landfill sites is -58 +/- 3%o. The delta C-13-CH4 signature for gas leaks is also fairly constant around -36 +/- 2 parts per thousand, a value characteristic of homogenised North Sea supply. In contrast, signatures for coal mines in N. England and Wales fall in a range of -51.2 +/- 0.3 parts per thousand to 30.9 +/- 1.4 parts per thousand, but can be tightly constrained by region. The study demonstrates that CRDS-based mobile methane measurement coupled with off-line high precision isotopic analysis of plume samples is an efficient way of characterising methane sources. It shows that iiotopic measurements allow type identification, and possible location of previously unknown methane sources. In modelling studies this measurement provides an independent constraint to determine the contributions of different sources to the regional methane budget and in the verification of inventory source distribution. (C) 2015 Elsevier Ltd. All rights reserved

THERMODYNAMIC ANALYSIS OF SYNTHESIS GAS AND HIGHER HYDROCARBONS PRODUCTION FROM METHANE

This chapter focused on thermodynamic chemical equilibrium analysis using method of direct minimization of Gibbs free energy for all possible methane reactions with oxygen (partial oxidation of methane), carbon dioxide (CO2 reforming of methane), steam (steam reforming of methane), and autothermal reforming. Effects of feed ratios (methane to oxygen, carbon dioxide, and/or steam feed ratio), reaction temperature, and system pressure on equilibrium composition, conversion, and yield were studied. In addition, operating regions of carbon and no carbon formation were also considered at various reaction temperatures and feed ratios in the equilibrium system. It was found that the reaction temperature above 1100 K and CH4/CO2 ratio unity were favorable for synthesis gas production for methane – carbon dioxide reaction. The Carbon Dioxide Oxidative Coupling of Methane reaction to produce ethane and ethylene is less favorable thermodynamically. In addition, steam reforming of methane is the most suitable for hydrogen production from methane with low coke formation from thermodynamic point of view

Research progress on coal mine laser methane sensor

This paper discusses the research progress of low-power technology of laser methane sensors for coal mine. On the basis of environment of coal mines, such as ultra-long-distance transmission and high stability, a series of studies have been carried out. The preliminary results have been achieved in the research of low power consumption, temperature and pressure compensation and reliability design. The technology is applied to various products in coal mines, and achieves high stability and high reliability in products such as laser methane sensor, laser methane detection alarm device, wireless laser methane detection alarm device, and optic fiber multichannel laser methane sensor. Experimental testing and analysis of the characteristics of laser methane sensors, combined with the actual application

Microbial diversity and biogenic methane potential of a thermogenic-gas coal mine

The microbial communities and biogenic methane potential of a gas coal mine were investigated by cultivation-independent and cultivation-dependent approaches. Stable carbon isotopic analysis indicated that in situ methane in the coal mine was dominantly of a thermogenic origin. However, a high level of diversity of bacteria and methanogens that were present in the coal mine was revealed by 454 pyrosequencing, and included various fermentative bacteria in the phyla of Actinobacteria, Bacteroidetes, Firmicutes, and Proteobacteria, and acetotrophic, hydrogenotrophic, and methylotrophic methanogens. Methane was produced in enrichments of mine water samples supplemented with acetate under laboratory conditions. The microbial flora obtained from the enrichments could stimulate methane formation from coal samples. 16S rRNA gene clone library analysis indicated that the microbial community from coal cultivation samples supplemented with the enriched microbial consortium was dominated by the anaerobic fermentative Clostridiales and facultative acetoclastic Methanosarcina. This study suggests that the biogenic methane potential in the thermogenic-gas coal mine could be stimulated by the indigenous microorganisms

Methane emissions from the 2015 Aliso Canyon blowout in Los Angeles, CA.

Single-point failures of natural gas infrastructure can hamper methane emission control strategies designed to mitigate climate change. The 23 October 2015 blowout of a well connected to the Aliso Canyon underground storage facility in California resulted in a massive release of natural gas. Analysis of methane and ethane data from dozens of plume transects, collected during 13 research-aircraft flights between 7 November 2015 and 13 February 2016, shows atmospheric leak rates of up to 60 metric tons of methane and 4.5 metric tons of ethane per hour. At its peak, this blowout effectively doubled the methane emission rate of the entire Los Angeles basin and, in total, released 97,100 metric tons of methane to the atmosphere

TAP investigations of the CO2 reforming of CH4 over Pt/ZrO2

The adsorption and reaction characteristics of methane, carbon dioxide, carbon monoxide, and hydrogen have been investigated over a ZrO2support and a Pt/ZrO2catalyst by using a temporal analysis of products reactor system. It was observed that on Pt/ZrO2both methane and carbon dioxide dissociate independently of one another. The dissociation of carbon dioxide acts as an oxygen supplier, while the decomposition products of methane scavenge the oxygen from the catalyst. When an abundance of oxygen is present, pulsing of methane leads to the production of carbon dioxide. It is concluded that both the selectivity with which methane produces carbon monoxide or carbon dioxide and the carbon dioxide conversion is determined by the same reaction: COads+Oads CO2,ads

Methane and Nitrogen Abundances On Pluto and Eris

We present spectra of Eris from the MMT 6.5 meter telescope and Red Channel Spectrograph (5700-9800 angstroms; 5 angstroms per pix) on Mt. Hopkins, AZ, and of Pluto from the Steward Observatory 2.3 meter telescope and Boller and Chivens spectrograph (7100-9400 angstroms; 2 angstroms per pix) on Kitt Peak, AZ. In addition, we present laboratory transmission spectra of methane-nitrogen and methane-argon ice mixtures. By anchoring our analysis in methane and nitrogen solubilities in one another as expressed in the phase diagram of Prokhvatilov and Yantsevich (1983), and comparing methane bands in our Eris and Pluto spectra and methane bands in our laboratory spectra of methane and nitrogen ice mixtures, we find Eris' bulk methane and nitrogen abundances are about 10% and about 90%, and Pluto's bulk methane and nitrogen abundances are about 3% and about 97%. Such abundances for Pluto are consistent with values reported in the literature. It appears that the bulk volatile composition of Eris is similar to the bulk volatile composition of Pluto. Both objects appear to be dominated by nitrogen ice. Our analysis also suggests, unlike previous work reported in the literature, that the methane and nitrogen stoichiometry is constant with depth into the surface of Eris. Finally, we point out that our Eris spectrum is also consistent with a laboratory ice mixture consisting of 40% methane and 60% argon. Although we cannot rule out an argon rich surface, it seems more likely that nitrogen is the dominant species on Eris because the nitrogen ice 2.15 micron band is seen in spectra of Pluto and Triton.Comment: The manuscript has 44 pages, 15 figures, and four tables. It will appear in the Astrophysical Journa

Molecule mapping of HR8799b using OSIRIS on Keck: Strong detection of water and carbon monoxide, but no methane

Context. In 2015, Barman et al. (ApJ, 804, 61) presented detections of absorption from water, carbon monoxide, and methane in the atmosphere of the directly imaged exoplanet HR8799b using integral field spectroscopy (IFS) with OSIRIS on the Keck II telescope. We recently devised a new method to analyse IFU data, called molecule mapping, searching for high-frequency signatures of particular molecules in an IFU data cube. Aims. The aim of this paper is to use the molecule mapping technique to search for the previously detected spectral signatures in HR8799b using the same data, allowing a comparison of molecule mapping with previous methods. Methods. The medium-resolution H- and K-band pipeline-reduced archival data were retrieved from the Keck archive facility. Telluric and stellar lines were removed from each spectrum in the data cube, after which the residuals were cross-correlated with model spectra of carbon monoxide, water, and methane. Results. Both carbon monoxide and water are clearly detected at high signal-to-noise, however, methane is not retrieved. Conclusions. Molecule mapping works very well on the OSIRIS data of exoplanet HR8799b. However, it is not evident why methane is detected in the original analysis, but not with the molecule mapping technique. Possible causes could be the presence of telluric residuals, different spectral filtering techniques, or the use of different methane models. We do note that in the original analysis methane was only detected in the K-band, while the H-band methane signal could be expected to be comparably strong. More sensitive observations with the JWST will be capable of confirming or disproving the presence of methane in this planet at high confidence.Comment: 5 pages, 5 figures and 2 tables, accepted by A&

Pluto's lower atmosphere structure and methane abundance from high-resolution spectroscopy and stellar occultations

Context: Pluto possesses a thin atmosphere, primarily composed of nitrogen, in which the detection of methane has been reported. Aims: The goal is to constrain essential but so far unknown parameters of Pluto's atmosphere such as the surface pressure, lower atmosphere thermal stucture, and methane mixing ratio. Methods: We use high-resolution spectroscopic observations of gaseous methane, and a novel analysis of occultation light-curves. Results: We show that (i) Pluto's surface pressure is currently in the 6.5-24 microbar range (ii) the methane mixing ratio is 0.5+/-0.1 %, adequate to explain Pluto's inverted thermal structure and ~100 K upper atmosphere temperature (iii) a troposphere is not required by our data, but if present, it has a depth of at most 17 km, i.e. less than one pressure scale height; in this case methane is supersaturated in most of it. The atmospheric and bulk surface abundance of methane are strikingly similar, a possible consequence of the presence of a CH4-rich top surface layer.Comment: AA vers. 6.1, LaTeX class for Astronomy & Astrophysics, 9 pages with 5 figures Astronomy and Astrophysics Letters, in pres

Stable isotopic analysis of atmospheric methane by infrared spectroscopy by use of diode laser difference-frequency generation

An infrared absorption spectrometer has been constructed to measure the stable isotopic composition of atmospheric methane samples. The spectrometer employs periodically poled lithium niobate to generate 15 μW of tunable difference-frequency radiation from two near-infrared diode lasers that probe the ν3 rotational-vibrational band of methane at 3.4 μm. To enhance the signal, methane is extracted from 25 l of air by use of a cryogenic chromatographic column and is expanded into the multipass cell for analysis. A measurement precision of 12‰ is demonstrated for both δ13C and δD