Natural gas hydrates are solid, non-stoichiometric compounds of small gas molecules and water. They form when the constituents come into contact at low temperature and high pressure. The physical properties of these compounds, most notably that they are non-flowing crystalline solids that are denser than typical fluid hydrocarbons and that the gas molecules they contain are effectively compressed, give rise to numerous applications in the broad areas of energy and climate effects. In particular, they have an important bearing on flow assurance and safety issues in oil and gas pipelines, they offer a largely unexploited means of energy recovery and transportation, and they could play a significant role in past and future climate change.

Fundamental principles and applications of natural gas hydrates

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios-which differ in fossil fuel and microbial emissions-to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain. © 2013 Macmillan Publishers Limited.

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Three decades of global methane sources and sinks

Large, abrupt, and widespread climate changes with major impacts have occurred repeatedly in the past, when the Earth system was forced across thresholds. Although abrupt climate changes can occur for many reasons, it is conceivable that human forcing of climate change is increasing the probability of large, abrupt events. Were such an event to recur, the economic and ecological impacts could be large and potentially serious. Unpredictability exhibited near climate thresholds in simple models shows that some uncertainty will always be associated with projections. In light of these uncertainties, policy-makers should consider expanding research into abrupt climate change, improving monitoring systems, and taking actions designed to enhance the adaptability and resilience of ecosystems and economies.

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Abrupt climate change

Large amounts of methane are produced in marine sediments but are then consumed before contacting aerobic waters or the atmosphere1. Although no organism that can consume methane anaerobically has ever been isolated, biogeochemical evidence indicates that the overall process involves a transfer of electrons from methane to sulphate and is probably mediated by several organisms, including a methanogen (operating in reverse) and a sulphate-reducer (using an unknown intermediate substrate)2. Here we describe studies of sediments related to a decomposing methane hydrate. These provide strong evidence that methane is being consumed by archaebacteria that are phylogenetically distinct from known methanogens. Specifically, lipid biomarkers that are commonly characteristic of archaea are so strongly depleted in carbon-13 that methane must be the carbon source, rather than the metabolic product, for the organisms that have produced them. Parallel gene surveys of small-subunit ribosomal RNA (16S rRNA) indicate the predominance of a new archael group which is peripherally related to the methanogenic orders Methanomicrobiales and Methanosarcinales.

Methane-consuming archaebacteria in marine sediments

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations).

For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30∘ N) compared to mid-latitudes (∼ 30 %, 30–60∘ N) and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters.

Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning.

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The global methane budget 2000–2017

The continental margin off Prins Karls Forland, western Svalbard, is characterized by widespread natural gas seepage into the water column at and upslope of the gas hydrate stability zone. We deployed an ocean bottom seismometer integrated into the MASOX (Monitoring Arctic Seafloor-Ocean Exchange) automated seabed observatory at the pinch-out of this zone at 389 m water depth to investigate passive seismicity over a continuous 297 day period from 13 October 2010. An automated triggering algorithm was applied to detect over 220,000 short duration events (SDEs) defined as having a duration of less than 1 s. The analysis reveals two different types of SDEs, each with a distinctive characteristic seismic signature. We infer that the first type consists of vocal signals generated by moving mammals, likely finback whales. The second type corresponds to signals with a source within a few hundred meters of the seismometer, either due east or west, that vary on short (∼tens of days) and seasonal time scales. Based on evidence of prevalent seafloor seepage and subseafloor gas accumulations, we hypothesize that the second type of SDEs is related to subseafloor fluid migration and gas seepage. Furthermore, we postulate that the observed temporal variations in microseismicity are driven by transient fluid release and due to the dynamics of thermally forced, seasonal gas hydrate decomposition. Our analysis presents a novel technique for monitoring the duration, intensity, and periodicity of fluid migration and seepage at the seabed and can help elucidate the environmental controls on gas hydrate decomposition and release.

https://agupubs.onlinelibrary.wiley.com/doi/epdf/10.1002/2017GC007107

Microseismicity Linked to Gas Migration and Leakage on the Western Svalbard Shelf

Submarine Landslides on Continental Margins

. Methane ( CH4 ) in marine sediments has the potential
to contribute to changes in the ocean and climate system. Physical and
biochemical processes that are difficult to quantify with current standard
methods such as acoustic surveys and discrete sampling govern the
distribution of dissolved CH4 in oceans and lakes. Detailed
observations of aquatic CH4 concentrations are required for a better understanding of CH4 dynamics in the water column, how it can affect lake and ocean acidification, the chemosynthetic ecosystem, and mixing ratios of atmospheric climate gases. Here we present pioneering
high-resolution in situ measurements of dissolved CH4 throughout the water column over a 400 m deep CH4 seepage area at the continental slope west of Svalbard. A new fast-response underwater membrane-inlet laser spectrometer sensor demonstrates technological advances and breakthroughs for ocean measurements. We reveal decametre-scale variations in dissolved CH4 concentrations over the CH4 seepage zone. Previous studies could not resolve such heterogeneity in the area, assumed a smoother distribution, and therefore lacked both details on and insights into ongoing processes. We show good repeatability of the instrument measurements, which are also in agreement with discrete sampling. New numerical models, based on acoustically evidenced free gas emissions from the seafloor, support the observed heterogeneity and CH4 inventory. We identified sources of CH4 , undetectable with echo sounder, and rapid diffusion of dissolved CH4 away from the sources. Results from the continuous ocean laser-spectrometer measurements, supported by modelling, improve our
understanding of CH4 fluxes and related physical processes over Arctic CH4 degassing regions.

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High-resolution underwater laser spectrometer sensing provides new insights into methane distribution at an Arctic seepage site

MOCA—Methane Emissions from the Arctic OCean to the Atmosphere: Present and Future Climate Effects is funded by the Research Council of Norway, grant 225814. CAGE—Centre for Arctic Gas Hydrate, Environment and Climate research work was supported by the Research Council of Norway through its Centres of Excellence funding scheme grant 223259. eSTICC—eScience Tools for Investigating Climate Change in northern high latitudes is supported by Nordforsk as Nordic Center of Excellence grant 57001. NERC grants NE/I029293/1 (PI. H. Coe) and NE/I02916/1 (PI J. Pyle) and Methane & Other Greenhouse Gases in the Arctic—Measurements, Process Studies and Modelling (MAMM). The ERC through the ACCI project, project number 267760. The biogenic methane emission data from the LPX-Bern v1.2 model were provided by Renato Spahni. The methane emission data from the GAINS model were provided by IIASA. GFED data are available from http://www.globalfiredata.org/index.html. Airborne data were obtained using the BAe-146-301 Atmospheric Research Aircraft (ARA) flown by Directflight Ltd. and managed by the Facility for Airborne Atmospheric Measurements (FAAM), which is a joint entity of the Natural Environment Research Council (NERC) and the Met Office. Zeppelin and Helmer Hansen atmospheric measurement data are archived in EBAS (http://ebas.nilu.no/) for long-term preservation, access and use. All Zeppelin data for 2014: http://ebas.nilu.no/DataSets.aspx?stations=NO0042G&fromDate=2014-01-01&toDate=2014-12-31. All atmospheric data from RV Helmer Hanssen: http://ebas.nilu.no/DataSets.aspx?stations=NO1000R&fromDate=2014-01-01&toDate=2014-12-31 (password is required until the end of 2017).

https://www.research.manchester.ac.uk/portal/files/49526750/Pisso_et_al_2016_Constraints_on_oceanic_methane_emissions_west_of_Svalbard_from_atmospheric_in_situ_measurements_and_Lagrangian_tra.pdf

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling.

Deep sea sediment cores taken between 50° and 75°N in the North Atlantic, in water depths varying between 1340 and 3850 m, were examined to provide an astronomically calibrated late Quaternary time-scale based on physical property records. Magnetic susceptibility and gamma ray attenuation porosity evaluator (GRAPE) density changes of these cores revealed significant responses to orbital forcing in the eccentricity (100 kyr), obliquity (41 kyr) and precessional (23, 19 kyr) bands. At 75°N (Greenland Sea), a response to obliquity forcing was weak despite the fact that it should become more pronounced in sediments at high latitudes. Application of bandpass filtering at the obliquity period (41 kyr), however, showed that variance at this period did exist in the magnetic susceptibility record, but at a very low power. At 50°N stacked curves of magnetic susceptibility correlated strongly with the SPECMAP curve for the past 500 ka. Since about 65 ka, dropstone layers are recorded in both magnetic susceptibility and GRAPE data of Rockall Plateau sediments. Although Rockall Plateau sediments show peaks in physical properties that correlate with Heinrich events (H1, H2, H4, H5, H6), such a relationship was not readily observed in Norwegian-Greenland Sea records. Heinrich events at Rockall Plateau sites indicate a northward flow of icebergs in the eastern North Atlantic. This flow pattern and the presence of Heinrich events during the past 65 ka raise the questions of whether similar events occurred before this time period, and to what kind of ice sheet dynamics and climatic-oceanographic conditions favoured major iceberg surges from the Laurentide ice sheet to the North Atlantic at 50°N.

Jürgen Mienert

Papers

Microseismicity Linked to Gas Migration and Leakage on the Western Svalbard Shelf

Submarine Landslides on Continental Margins

High-resolution underwater laser spectrometer sensing provides new insights into methane distribution at an Arctic seepage site

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling.

Astronomical time-scale for physical property records from Quaternary sediments of the northern North Atlantic