M. Lanoisellé

Escape of methane gas from the seabed along the West Spitsbergen continental margin

More than 250 plumes of gas bubbles have been discovered emanating from the seabed of the West Spitsbergen continental margin, in a depth range of 150-400 m, at and above the present upper limit of the gas hydrate stability zone (GHSZ). Some of the plumes extend upward to within 50 m of the sea surface. The gas is predominantly methane. Warming of the northward-flowing West Spitsbergen current by 1°C over the last thirty years is likely to have increased the release of methane from the seabed by reducing the extent of the GHSZ, causing the liberation of methane from decomposing hydrate. If this process becomes widespread along Arctic continental margins, tens of Teragrams of methane per year could be released into the ocean.

Arctic methane sources: Isotopic evidence for atmospheric inputs

By comparison of the methane mixing ratio and the carbon isotope ratio (δ13CCH4) in Arctic air with regional background, the incremental input of CH4 in an air parcel and the source δ13CCH4 signature can be determined. Using this technique the bulk Arctic CH4 source signature of air arriving at Spitsbergen in late summer 2008 and 2009 was found to be −68‰, indicative of the dominance of a biogenic CH4 source. This is close to the source signature of CH4 emissions from boreal wetlands. In spring, when wetland was frozen, the CH4 source signature was more enriched in 13C at −53 ± 6‰ with air mass back trajectories indicating a large influence from gas field emissions in the Ob River region. Emissions of CH4 to the water column from the seabed on the Spitsbergen continental slope are occurring but none has yet been detected reaching the atmosphere. The measurements illustrate the significance of wetland emissions. Potentially, these may respond quickly and powerfully to meteorological variations and to sustained climate warming.

Rising atmospheric methane: 2007-2014 growth and isotopic shift

From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7 ± 1.2 ppb yr−1. Simultaneously, δ13CCH4 (a measure of the 13C/12C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5 ± 0.4 ppb, with a further shift to more negative values being observed at most latitudes. The isotopic evidence presented here suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies. Changes in the removal rate of methane by the OH radical have not been seen in other tracers of atmospheric chemistry and do not appear to explain short-term variations in methane. Fossil fuel emissions may also have grown, but the sustained shift to more 13C-depleted values and its significant interannual variability, and the tropical and Southern Hemisphere loci of post-2007 growth, both indicate that fossil fuel emissions have not been the dominant factor driving the increase. A major cause of increased tropical wetland and tropical agricultural methane emissions, the likely major contributors to growth, may be their responses to meteorological change.

Measurement of the 13C isotopic signature of methane emissions from northern European wetlands

Isotopic data provide powerful constraints on regional and global methane emissions and their source profiles. However, inverse modeling of spatially resolved methane flux is currently constrained by a lack of information on the variability of source isotopic signatures. In this study, isotopic signatures of emissions in the Fennoscandian Arctic have been determined in chambers over wetland, in the air 0.3 to 3 m above the wetland surface and by aircraft sampling from 100 m above wetlands up to the stratosphere. Overall, the methane flux to atmosphere has a coherent δ13C isotopic signature of −71 ± 1‰, measured in situ on the ground in wetlands. This is in close agreement with δ13C isotopic signatures of local and regional methane increments measured by aircraft campaigns flying through air masses containing elevated methane mole fractions. In contrast, results from wetlands in Canadian boreal forest farther south gave isotopic signatures of −67 ± 1‰. Wetland emissions dominate the local methane source measured over the European Arctic in summer. Chamber measurements demonstrate a highly variable methane flux and isotopic signature, but the results from air sampling within wetland areas show that emissions mix rapidly immediately above the wetland surface and methane emissions reaching the wider atmosphere do indeed have strongly coherent C isotope signatures. The study suggests that for boreal wetlands (>60°N) global and regional modeling can use an isotopic signature of −71‰ to apportion sources more accurately, but there is much need for further measurements over other wetlands regions to verify this.

Measurements of δ13C in CH4 and using particle dispersion modeling to characterize sources of arctic methane within an air mass

Abstract A stratified air mass enriched in methane (CH4) was sampled at ~600 m to ~2000 m altitude, between the north coast of Norway and Svalbard as part of the Methane in the Arctic: Measurements and Modelling campaign on board the UKs BAe‐146‐301 Atmospheric Research Aircraft. The approach used here, which combines interpretation of multiple tracers with transport modeling, enables better understanding of the emission sources that contribute to the background mixing ratios of CH4 in the Arctic. Importantly, it allows constraints to be placed on the location and isotopic bulk signature of the emission source(s). Measurements of δ13C in CH4 in whole air samples taken while traversing the air mass identified that the source(s) had a strongly depleted bulk δ13C CH4 isotopic signature of −70 (±2.1)‰. Combined Numerical Atmospheric‐dispersion Modeling Environment and inventory analysis indicates that the air mass was recently in the planetary boundary layer over northwest Russia and the Barents Sea, with the likely dominant source of methane being from wetlands in that region.

Evaluating methane inventories by isotopic analysis in the London region

A thorough understanding of methane sources is necessary to accomplish methane reduction targets. Urban environments, where a large variety of methane sources coexist, are one of the most complex areas to investigate. Methane sources are characterised by specific δ13C-CH4 signatures, so high precision stable isotope analysis of atmospheric methane can be used to give a better understanding of urban sources and their partition in a source mix. Diurnal measurements of methane and carbon dioxide mole fraction, and isotopic values at King’s College London, enabled assessment of the isotopic signal of the source mix in central London. Surveys with a mobile measurement system in the London region were also carried out for detection of methane plumes at near ground level, in order to evaluate the spatial allocation of sources suggested by the inventories. The measured isotopic signal in central London (−45.7 ±0.5‰) was more than 2‰ higher than the isotopic value calculated using emission inventories and updated δ13C-CH4 signatures. Besides, during the mobile surveys, many gas leaks were identified that are not included in the inventories. This suggests that a revision of the source distribution given by the emission inventories is needed.

A cautionary tale: A study of a methane enhancement over the North Sea

Airborne measurements of a methane (CH4) plume over the North Sea from August 2013 are analyzed. The plume was only observed downwind of circumnavigated gas fields, and three methods are used to determine its source. First, a mass balance calculation assuming a gas field source gives a CH4 emission rate between 2.5±0.8x104 and 4.6±1.5x104 kg h−1. This would be greater than the industry target of a 0.5% leak rate if it were emitting for more than half the time. Second, annual average UK CH4 emissions are combined with an atmospheric dispersion model to create pseudo-observations. Clean air from the North Atlantic passed over mainland UK, picking up anthropogenic emissions. To best explain the observed plume using pseudo-observations, an additional North Sea source from the gas rigs area is added. Third, the δ13C-CH4 from the plume is shown to be -53%0, which is lighter than fossil gas but heavier than the UK average emission. We conclude that either an additional small-area mainland source is needed, combined with temporal variability in emission or transport in small-scale meteorological features. Alternatively, a combination of additional sources that are at least 75% from the mainland (-58%0) and up to 25% from the North Sea gas rigs area (-32%0) would explain the measurements. Had the isotopic analysis not been performed, the likely conclusion would have been of a gas field source of CH4. This demonstrates the limitation of analysing mole fractions alone, as the simplest explanation is rejected based on analysis of isotopic data.

Isotopic Ratios of Tropical Methane Emissions by Atmospheric Measurement

Tropical methane sources are an important part of the global methane budget and include natural wetlands, rice agriculture, biomass burning, ruminants, fossil fuels, and waste. δ13CCH4 can provide strong constraints on methane source apportionment. For example, tropical wetlands in this study give δ13CCH4 values between −61.5 ± 2.9‰ and −53.0 ± 0.4‰ and in general are more enriched in 13C than temperate and boreal wetlands. However, thus far, relatively few measurements of δ13CCH4 in methane-enriched air have been made in the tropics. In this study samples have been collected from tropical wetland, rice, ruminant, and biomass burning emissions to the atmosphere. Regional isotopic signatures vary greatly as different processes and source material affect methane signatures. Measurements were made to determine bulk source inputs to the atmosphere, rather than to study individual processes. These measurements provide inputs for regional methane budget models, to constrain emissions with better source apportionment.

Marked long-term decline in ambient CO mixing ratio in SE England, 1997-2014: evidence of policy success in improving air quality

Atmospheric CO at Egham in SE England has shown a marked and progressive decline since 1997, following adoption of strict controls on emissions. The Egham site is uniquely positioned to allow both assessment and comparison of ‘clean Atlantic background’ air and CO-enriched air downwind from the London conurbation. The decline is strongest (approximately 50 ppb per year) in the 1997–2003 period but continues post 2003. A ‘local CO increment’ can be identified as the residual after subtraction of contemporary background Atlantic CO mixing ratios from measured values at Egham. This increment, which is primarily from regional sources (during anticyclonic or northerly winds) or from the European continent (with easterly air mass origins), has significant seasonality, but overall has declined steadily since 1997. On many days of the year CO measured at Egham is now not far above Atlantic background levels measured at Mace Head (Ireland). The results are consistent with MOPITT satellite observations and ‘bottom-up’ inventory results. Comparison with urban and regional background CO mixing ratios in Hong Kong demonstrates the importance of regional, as opposed to local reduction of CO emission. The Egham record implies that controls on emissions subsequent to legislation have been extremely successful in the UK.