scholarly journals Carbon isotopic signature of coal-derived methane emissions to atmosphere: from coalification to alteration

Author(s):  
Giulia Zazzeri ◽  
Dave Lowry ◽  
Rebecca E. Fisher ◽  
James France ◽  
Mathias Lanoisellé ◽  
...  

Abstract. Currently, the atmospheric methane burden is rising rapidly, but the extent to which shifts in coal production contribute to this rise is not known. Coalbed methane emissions into the atmosphere are poorly characterised, and this study provides representative δ13CCH4 signatures to be used in regional and global models in order to allow better apportionment of fossil fuel emissions. Integrated methane emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised. Progression in coal rank and secondary biogenic production of methane due to incursion of water are suggested as the processes affecting the isotopic composition of coal-derived methane. An averaged value of −65 ‰ has been assigned to bituminous coal exploited in open cast mines and of −55 ‰ in deep mines, whereas values of −40 ‰ and −30 ‰ can be allocated to anthracite opencast and deep mines respectively. However, the isotopic signatures that are included in global atmospheric modelling of coal emissions should be region or nation specific, as greater detail is needed, given the wide global variation in coal type.

2016 ◽  
Vol 16 (21) ◽  
pp. 13669-13680 ◽  
Author(s):  
Giulia Zazzeri ◽  
Dave Lowry ◽  
Rebecca E. Fisher ◽  
James L. France ◽  
Mathias Lanoisellé ◽  
...  

Abstract. Currently, the atmospheric methane burden is rising rapidly, but the extent to which shifts in coal production contribute to this rise is not known. Coalbed methane emissions into the atmosphere are poorly characterised, and this study provides representative δ13CCH4 signatures of methane emissions from specific coalfields. Integrated methane emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised. Progression in coal rank and secondary biogenic production of methane due to incursion of water are suggested as the processes affecting the isotopic composition of coal-derived methane. An averaged value of −65 ‰ has been assigned to bituminous coal exploited in open cast mines and of −55 ‰ in deep mines, whereas values of −40 and −30 ‰ can be allocated to anthracite opencast and deep mines respectively. However, the isotopic signatures that are included in global atmospheric modelling of coal emissions should be region- or nation-specific, as greater detail is needed, given the wide global variation in coal type.


2021 ◽  
Author(s):  
Semra Bakkaloglu ◽  
Dave Lowry ◽  
Rebecca Fisher ◽  
James France ◽  
Euan Nisbet

<p>Biological methane oxidation in landfill cover material can be characterised using stable isotopes. Methane oxidation fraction is calculated from the carbon isotopic signature of emitted CH<sub>4</sub>, with enhanced microbial consumption of methane in the aerobic portion of the landfill cover indicated by a shift to less depleted isotopic values in the residual methane emitted to air. This study was performed at four southwest England landfill sites. Mobile mole fraction measurement at the four sites was coupled with Flexfoil bag sampling of air for high-precision isotope analysis. Gas well samples collected from the pipeline systems and downwind plume air samples were utilized to estimate methane oxidation rate for whole sites. This work was designed to assess the impact on carbon isotopic signature and oxidation rate as UK landfill practice and waste streams have changed in recent years.</p><p>The landfill status such as closed and active, seasonal variation, cap stripping and site closure impact on landfill isotopic signature and oxidation rate were evaluated. The isotopic signature of <sup>13</sup>C-CH<sub>4</sub> values of emissions varied between -60 and -54‰, with an averaged value of -57 +- 2‰ for methane from closed and active landfill sites. Methane emissions from older, closed landfill sites were typically more enriched in <sup>13</sup>C than emissions from active sites. This study found that the isotopic signature of <sup>13</sup>C-CH<sub>4</sub> of fugitive methane did not show a seasonal trend, and there was no plume observed from a partial cap stripping process to assess changes in <sup>13</sup>C-CH<sub>4</sub>  isotopic signatures of emitted methane. Also, the closure of an active landfill cell caused a significant decrease in mole fraction of measured CH<sub>4</sub>, which was less depleted <sup>13</sup>C in the emitted plume due to a higher oxidation rate. Methane oxidation, estimated from the isotope fractionation, ranged from 3 to 27%, with mean values of 7% and 15% for active and closed landfills, respectively. These results indicate that the oxidation rate is highly site specific.</p><p> </p>


2021 ◽  
Author(s):  
Alina Fiehn ◽  
Julian Kostinek ◽  
Maximilian Eckl ◽  
Michal Galkowski ◽  
Christoph Gerbig ◽  
...  

<p>Emissions from fossil fuels are one of the primary sources of atmospheric methane (CH<sub>4</sub>) growth. However, estimates of anthropogenic CH<sub>4</sub> emissions still show large uncertainties on global and regional scales. Differences in CH<sub>4</sub> isotopic source signatures δ<sup>13</sup>C and δD can help to constrain different source contributions (e.g. fossil, thermogenic, or biogenic).</p><p>The Upper Silesian Coal Basin (USCB) represents one of the largest European CH<sub>4</sub> emission source regions, with more than 500 Gg CH<sub>4</sub> yr<sup>-1</sup> released by more than 50 coal mine ventilation shafts. During the CoMet (Carbon Dioxide and Methane Mission) campaign in June 2018 methane observations were conducted from a variety of platforms including aircraft and cars. Beside the continuous sampling of atmospheric methane concentration, numerous air samples were taken from inside the ventilation shafts, around the ventilation shafts (1‑2 km distance) and aboard the DLR Cessna Caravan aircraft and analyzed in the laboratory for the isotopic composition of CH<sub>4</sub>.</p><p>The ground-based samples allowed determining the source signatures of individual ventilation shafts. These signatures displayed a considerable range between different shafts and also varied from day to day. The airborne samples contained a mixture of methane emissions from several mines and thus enabled accurately determining the signature of the entire region. The mean isotopic signature of methane emissions over the USCB derived from the aircraft samples was -51.9 ± 0.5 ‰ for δ<sup>13</sup>C and -233 ± 6 ‰ for δD. This is in between the range of other microbial and thermogenic coal reservoirs, but more depleted in δD than previous USCB studies reported based on samples taken within the mines. Signatures of methane enhancements sampled upwind of the mines and in the free troposphere clearly showed the presence of methane of biogenic origin (e.g. wetlands, waste, ruminants).</p><p>Furthermore, we simulated the methane isotopologues using the on-line three-times nested global regional chemistry climate model MECO(n). We implemented a submodel extension, which includes the kinetic fractionation and uses the isotopic source signatures determined by the ground-based observations. We compare the regional simulations to flask samples taken during CoMet.</p>


1995 ◽  
Vol 35 (1) ◽  
pp. 613 ◽  
Author(s):  
R. E. Summons ◽  
C. J. Boreham ◽  
C. B. Foster ◽  
A. P. Murray ◽  
J. D. Gorter

The known global secular change in the distribu­tion of carbon isotopes between the Palaeozoic and Mesozoic is the basis of a new oil-source correlation tool. The carbon isotopic signatures of n-alkanes, in combination with information about the distribu­tions of diagnostic biomarkers have been used to classify Perth Basin oils according to the age of the source. These data confirm that most of the oil in the northern Perth Basin originates from the basal section of the Kockatea Shale.Oils exclusively from Triassic sources are isotopically light with n-alkane 813C values near −34%o PDB. Jurassic oil from Gage Roads-1 is isotopically heavy (~24%o) and is also distinctive in its relatively high content of conifer-derived aromatic hydrocar­bons. Condensates from Jurassic source intervals in the Dandaragan Trough are isotopically heteroge­neous with n-alkane 813C values between −25%o and −29%o. The Whicher Range-1 condensate, of appar­ent Permian origin, is isotopically heavy with n-alkane 5l3C values near −25%o. The isotopic data provide information about variation in sedimen­tary facies and possible multiple sources that is not evident from the biomarker signatures. All the Jurassic oils have significant amounts of bicadinanes, resin-derived biomarkers until recently attributed exclusively to tropical angiosperms.A strong excursion in the isotopic signature of organic carbon is present in core at 2,293 m in the Woodada-2 borehole and occurs with no obvious lithological change. Similar isotope shifts are known to mark the Permian-Triassic boundary globally and have been previously recognised in the Bonaparte, Bowen, Canning, Carnarvon and tenta­tively in the southern Perth basins. The excursion in Woodada-2 is abrupt and suggests a significant time break in sedimentation. However, diagnostic Permian palynoflora or fauna have not been de­tected below 2,293 m in the Woodada-2 core, and hence, the assignment of a Permian-Triassic con­tact cannot be made unequivocally with the exist­ing data.


Eos ◽  
2017 ◽  
Author(s):  
Terri Cook

Aircraft measurements confirm that methane emissions from northern European wetlands exhibit a uniform regional carbon isotopic signature, despite considerable ground-level heterogeneity.


2018 ◽  
Author(s):  
Sarah Connors ◽  
Alistair J. Manning ◽  
Andrew D. Robinson ◽  
Stuart N. Riddick ◽  
Grant L. Forster ◽  
...  

Abstract. Methane is a strong contributor to global climate change, yet our current understanding and quantification of its sources and their variability is incomplete. There is a growing need for comparisons between emission estimates produced using bottom-up inventory approaches and top-down inversion techniques based on atmospheric measurements, especially at higher spatial resolutions. To meet this need, this study presents using an inversion approach based on the Inversion Technique for Emissions Modelling (InTEM) framework and measurements from four sites in East Anglia, United Kingdom. Atmospheric methane concentrations were recorded at 1–2 minute time-steps at each location within the region of interest. These observations, coupled with the UK Met Office's Lagrangian particle dispersion model, NAME (Numerical Atmospheric dispersion Modelling Environment), were used within InTEM2014 to produce methane emission estimates for a 1-year period (June 2013–May 2014) in this eastern region of the UK (~ 100 × 150 km) at high spatial resolution (up to 4 × 4 km). InTEM2014 was able to produce realistic emissions estimates for East Anglia, and highlighted potential areas of difference from the UK National Atmospheric Emissions Inventory (NAEI). As this study was part of the UK Greenhouse gAs Uk and Global Emissions (GAUGE) project, observations were included within a national inversion using all eleven measurement sites across the UK to directly compare emission estimates for the East Anglia Region. Results show similar methane estimates for the East Anglia region. Methane emissions from Norfolk and Suffolk show good agreement with the estimates in NAEI, with differences of ~ 5 %. Larger differences are found for Cambridgeshire where our estimate is 22.5 % lower than that of NAEI. The addition of the EA sites within the national inversion system enabled finer spatial resolution and a decrease in the associated uncertainty for that area. Further development of our approach to include a more robust analysis of the methane concentration in the air entering this region and the uncertainty associated with the resulting emissions would strengthen this inverse method. Nonetheless, our results show there is value in high spatial resolution measurement networks and the resulting inversion emission estimates.


2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Henrik Drake ◽  
Nick M. W. Roberts ◽  
Manuel Reinhardt ◽  
Martin Whitehouse ◽  
Magnus Ivarsson ◽  
...  

AbstractEarth’s crust contains a substantial proportion of global biomass, hosting microbial life up to several kilometers depth. Yet, knowledge of the evolution and extent of life in this environment remains elusive and patchy. Here we present isotopic, molecular and morphological signatures for deep ancient life in vein mineral specimens from mines distributed across the Precambrian Fennoscandian shield. Stable carbon isotopic signatures of calcite indicate microbial methanogenesis. In addition, sulfur isotope variability in pyrite, supported by stable carbon isotopic signatures of methyl-branched fatty acids, suggest subsequent bacterial sulfate reduction. Carbonate geochronology constrains the timing of these processes to the Cenozoic. We suggest that signatures of an ancient deep biosphere and long-term microbial activity are present throughout this shield. We suggest that microbes may have been active in the continental igneous crust over geological timescales, and that subsurface investigations may be valuable in the search for extra-terrestrial life.


Molecules ◽  
2021 ◽  
Vol 26 (13) ◽  
pp. 3895
Author(s):  
Marica Baldoni ◽  
Alessandra Nardi ◽  
Flavio De Angelis ◽  
Olga Rickards ◽  
Cristina Martínez-Labarga

The present research investigates the relationship between dietary habits and mortality patterns in the Roman Imperial and Medieval periods. The reconstructions of population dynamics and subsistence strategies provide a fascinating source of information for understanding our history. This is particularly true given that the changes in social, economic, political, and religious aspects related to the transition from the Roman period to the Middle Ages have been widely discussed. We analyzed the isotopic and mortality patterns of 616 individuals from 18 archeological sites (the Medieval Latium sites of Colonna, Santa Severa, Allumiere, Cencelle, and 14 Medieval and Imperial funerary contexts from Rome) to compile a survivorship analysis. A semi-parametric approach was applied, suggesting variations in mortality patterns between sexes in the Roman period. Nitrogen isotopic signatures influenced mortality in both periods, showing a quadratic and a linear effect for Roman Imperial and Medieval populations, respectively. No influence of carbon isotopic signatures has been detected for Roman Imperial populations. Conversely, increased mortality risk for rising carbon isotopic values was observed in Medieval samples.


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