Microbial methane from in situ biodegradation of coal and shale: A review and reevaluation of hydrogen and carbon isotope signatures

Vinson, David S.; Blair, Neal E.; Martini, Anna M.; Larter, Stephen R.; Orem, William H.; McIntosh, Jennifer C.

doi:10.1016/j.chemgeo.2017.01.027

Cited by 121 publications

(93 citation statements)

References 156 publications

(301 reference statements)

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“…The fully-kinetic endmember is related to high H 2 concentrations (which yield a very large (negative) ∆ r G) (Burke, 1993). Therefore, hydrogenotrophic methanogens could produce CH 4 with isotopic signatures indistinguishable from those typically attributed to methylotrophic or acetoclastic methanogenesis (Whiticar, 1990;Vinson et al, 2017). Whether this is true will require evaluation by experiments under low H 2 conditions (Valentine et al, 2004;Kawagucci et al, 2014;Okumura et al, 2016) or in vitro (Scheller et al, 2013).…”

Section: Discussionmentioning

confidence: 99%

The geochemistry of methane isotopologues

Wang¹

2017

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This thesis documents the origin, distribution, and fate of methane and several of its isotopic forms on Earth. Using observational, experimental, and theoretical approaches, I illustrate how the relative abundances of 12 CH 4 , 13 CH 4 , 12 CH 3 D, and 13 CH 3 D record the formation, transport, and breakdown of methane in selected settings.Chapter 2 reports precise determinations of 13 CH 3 D, a "clumped" isotopologue of methane, in samples collected from various settings representing many of the major sources and reservoirs of methane on Earth. The results show that the information encoded by the abundance of 13 CH 3 D enables differentiation of methane generated by microbial, thermogenic, and abiogenic processes. A strong correlation between clumped-and hydrogen-isotope signatures in microbial methane is identified and quantitatively linked to the availability of H 2 and the reversibility of microbially-mediated methanogenesis in the environment. Determination of 13 CH 3 D in combination with hydrogen-isotope ratios of methane and water provides a sensitive indicator of the extent of C-H bond equilibration, enables fingerprinting of methane-generating mechanisms, and in some cases, supplies direct constraints for locating the waters from which migrated gases were sourced. Chapter 3 applies this concept to constrain the origin of methane in hydrothermal fluids from sediment-poor vent fields hosted in mafic and ultramafic rocks on slow-and ultraslow-spreading mid-ocean ridges. The data support a hypogene model whereby methane forms abiotically within plutonic rocks of the oceanic crust at temperatures above ca. 300• C during respeciation of magmatic volatiles, and is subsequently extracted during active, convective hydrothermal circulation. Chapter 4 presents the results of culture experiments in which methane is oxidized in the presence of O 2 by the bacterium Methylococcus capsulatus strain Bath. The results show that the clumped isotopologue abundances of partially-oxidized methane can be predicted from knowledge of 13 C/ 12 C and D/H isotope fractionation factors alone.: Shuhei Ono, Ph.D. Acknowledgments I fear that this section will not do justice to the people I have not the space to thank individually. Alas, here goes. To those whose names are not specifically listed here, thank you too. I wish first to thank Shuhei Ono. The work this thesis represents could not have happened without his bold vision and the license to explore and question that working in his lab afforded. His unbridled optimism, breadth of scientific curiosity, personal integrity, and accessibility to his personnel are traits I one day hope to emulate. I thank him for his nonjudgmental yet appropriately measured support of many of my ideas-even those that led nowhere-, for believing in me even when I found it difficult to do so myself, and for teaching me to change pump oil, build vacuum lines, and drink Icelandic vodka.I also wish to thank my thesis committee members Jeff Seewald, Roger Summons, and John Pohlman, for their in...

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Section: Discussionmentioning

confidence: 99%

The geochemistry of methane isotopologues

Wang¹

2017

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“…Although CBM production from coals in the Illinois Basin is small, CBM wells have been producing gas in Indiana and Illinois for more than 30 years, with Indiana's Sullivan County being the main CBM producing area in the basin [2,10]. A particularly useful diagnostic tool for the origin and possible microbial degradation of methane in natural gas are compound-specific hydrogen and carbon stable isotope ratios [11,12] that have also been employed in our study area [4,6].…”

Section: Introductionmentioning

confidence: 99%

Characteristics of Microbial Coalbed Gas during Production; Example from Pennsylvanian Coals in Indiana, USA

2017

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Coalbed gases from 11 wells producing from the Springfield and Seelyville Coal Members (Pennsylvanian) were analyzed for composition and carbon and hydrogen stable isotope ratios in four sampling events to investigate short-term variation trends. Nine wells in the Seelyville Coal Member produce coalbed gases from the virgin seam, whereas two wells in the Springfield Coal Member produce gas from mine voids. Methane dominates gas composition in all wells, and its content ranges from~94% to almost 98%, with ethane typically accounting for less than 0.01%. Carbon dioxide content in most samples is below 1%, whereas N 2 content ranges from less than 2% to 4.8%. Methane δ 13 C values range from −55.3‰ to −61.1‰, and δ 2 H values range from −201‰ to −219‰. Isotopic values of methane and C 1 /(C 2 + C 3 ) ratios indicate a biogenic origin along the CO 2 -reduction pathway, consistent with previous studies in this area. Our results demonstrate that gas properties may change significantly during a period of one year of production history. Compositional trends (e.g., C 1 /(C 2 + C 3 ), CH 4 /CO 2 ratios) are specific for each well and often irregular. These changes result from a combined influence of numerous factors and, therefore, are difficult to predict.

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“…αc is used in conjunction with αD to qualitatively characterise methanogenic environments indicated in The investigation into non-competitive substrates has expanded considerably, with methylotrophic methanogenesis being observed for Methanolobus by (Whitman et al, 2014). For mixed communities where there is sufficient concentrations of sulphate, iron (III) and nitrate, heterotrophic bacteria can aggressively outcompete methanogens for acetate, formate and H2 (Vinson et al, 2017). In the case of sulphate reducers, these substrates could be converted to CO2 and could shift the isotopic signature of the total pool in a different direction to the dominate methanogenesis mechanism.…”

Section: Stable Isotopes For Anaerobic Digestion In Landfill and Facumentioning

confidence: 99%

“…Vinson et al (2017) proposed a pathway-independent model to describe the proportion of organic carbon (CLMW) that is converted to CH4 (Figure 2-5). The system is simplified by grouping all methanogenesis and non-methanogenesis pathways in a simple, steady state isotope balance:…”

Section: Stable Isotopes For Anaerobic Digestion In Landfill and Facumentioning

confidence: 99%

“…(5-9) Vinson et al (2017) proposed partitioning the process of digestion into pathways which delineate CH4 production vs. other species, by defining a proportion 'f' to approximate the amount of substrate converted to CH4 vs CO2. This can be expressed in terms of a mass balance with isotope values, assuming all of the low molecular weight organic carbon substrate (CLMW) is produced and subsequently converted to CO2 or CH4: The δ 13 C-CLMW used for this study was adopted from previous classification of waste from the same facility and stage as -24.1‰ (Rafiee, 2016, Rafiee et al, 2017.…”

Section: Interpretation Of Stable Isotopesmentioning

confidence: 99%

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Aerobic processes in landfill: an Australian field trial

Obersky¹

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Modern landfills are often thought of as exclusively anaerobic systems, with landfill gas generation and regulatory emission models typically describing waste degradation as a first order decay process.However, in most instances, observed biogas production from landfills fall short of predictions by these landfill gas models. To improve biogas estimates, a closer examination of the configuration and operation of landfills is required, to identify if a significant portion of waste is degraded aerobically.An improved understanding of aerobic processes will contribute towards more accurate landfill gas estimation and emissions reporting.It was hypothesised that the rate and extent of anaerobic digestion (rAD), CH4 oxidation (rOX), and composting (rCOM) within the soil cover and the fresh waste immediately below the cover could be determined by the combination of stable isotope and molecular mass balances for carbon species (CH4 and CO2). The primary objective of this thesis was to determine the extent of simultaneous insitu aerobic (CH4 oxidation and composting) and anaerobic processes occurring in an operational landfill cell. An 18-month field trial was established on a fresh layer of waste placed on a sloped face at the edge of a landfill cell and covered with an interim soil cover (30-50cm).The evolution of CH4, CO2 and O2 through the waste profile and the surface emissions were monitored by gas samples collected from gas probes and static flux chambers. Stable isotopes ( 2 δH for CH4, 13 δC for CH4 and CO2) were monitored. The developed model consisted of four mass balances for CH4, CO2, δ 13 C-CH4 and δ 13 C-CO2 over a control volume that extended approximately 1.5m below the surface, incorporating the soil cover and the uppermost portion of the waste layer.The model was applied to data collected from two locations over four separate sampling campaigns, each representing a climatic season in Brisbane.It was necessary to conduct companion laboratory work to characterise key isotopic parameters in the model, these being (1) CH4 oxidation fractionation factor for the landfill cover soil, (2) anaerobic digestion fractionation factor for the waste, (3) the composting signature of the landfill cover and waste. The sensitivity of predictions of rAD, rCOM and rOX to the values of these parameters as well as the stoichiometry of the three reaction processes was assessed by randomly varying each parameter by ±5% over 500 simulations for each data set.iii The mass balance model revealed that aerobic activity forms a large proportion of early degradation

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Microbial methane from in situ biodegradation of coal and shale: A review and reevaluation of hydrogen and carbon isotope signatures

Cited by 121 publications

References 156 publications

The geochemistry of methane isotopologues

The geochemistry of methane isotopologues

Characteristics of Microbial Coalbed Gas during Production; Example from Pennsylvanian Coals in Indiana, USA

Aerobic processes in landfill: an Australian field trial

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