Abstract

Abstract. Methane (CH4) is a powerful greenhouse gas, whose natural and anthropogenic emissions contribute ∼20 % to global radiative forcing. Its atmospheric budget (sources and sinks), however, has large uncertainties. Inverse modelling, using atmospheric CH4 trends, spatial gradients and isotopic source signatures, has recently improved the major source estimates and their spatial–temporal variation. Nevertheless, isotopic data lack CH4 source representativeness for many sources, and their isotopic signatures are affected by incomplete knowledge of the spatial distribution of some sources, especially those related to fossil (radiocarbon-free) and microbial gas. This gap is particularly wide for geological CH4 (geo-CH4) seepage, i.e. the natural degassing of hydrocarbons from the Earth's crust. While geological seepage is widely considered a major source of atmospheric CH4, it has been largely neglected in 3-D inverse CH4 budget studies given the lack of detailed a priori gridded emission maps. Here, we report for the first time global gridded maps of geological CH4 sources, including emission and isotopic data. The 1∘×1∘ maps include the four main categories of natural geo-CH4 emission: (a) onshore hydrocarbon macro-seeps, including mud volcanoes, (b) submarine (offshore) seeps, (c) diffuse microseepage and (d) geothermal manifestations. An inventory of point sources and area sources was developed for each category, defining areal distribution (activity), CH4 fluxes (emission factors) and its stable C isotope composition (δ13C-CH4). These parameters were determined considering geological factors that control methane origin and seepage (e.g. petroleum fields, sedimentary basins, high heat flow regions, faults, seismicity). The global geo-source map reveals that the regions with the highest CH4 emissions are all located in the Northern Hemisphere, in North America, in the Caspian region, in Europe and in the East Siberian Arctic Shelf. The globally gridded CH4 emission estimate (37 Tg yr−1 exclusively based on data and modelling specifically targeted for gridding, and 43–50 Tg yr−1 when extrapolated to also account for onshore and submarine seeps with no location specific measurements available) is compatible with published ranges derived using top-down and bottom-up procedures. Improved activity and emission factor data allowed previously published mud volcanoes and microseepage emission estimates to be refined. The emission-weighted global mean δ13C-CH4 source signature of all geo-CH4 source categories is about −49 ‰. This value is significantly lower than those attributed so far in inverse studies to fossil fuel sources (−44 ‰) and geological seepage (−38 ‰). It is expected that using this updated, more 13C-depleted, isotopic signature in atmospheric modelling will increase the top-down estimate of the geological CH4 source. The geo-CH4 emission grid maps can now be used to improve atmospheric CH4 modelling, thereby improving the accuracy of the fossil fuel and microbial components. Grid csv (comma-separated values) files are available at https://doi.org/10.25925/4j3f-he27.

Highlights

  • Methane (CH4) is a powerful greenhouse gas, whose concentrations in the atmosphere have increased about 2.5 times since the pre-industrial era (1750), approaching 1.9 ppm in 2018

  • Global box modelling based on isotopic measurements of source signatures and the atmosphere combined with three-dimensional (3-D) forward modelling using trends and spatial gradients recently improved the knowledge of major sources and their spatial–temporal variation (e.g. Schwietzke et al, 2016)

  • Assuming that (a) submarine (offshore) seeps (SSs) generally do not take into account the release of dissolved methane and (b) today unknown SS areas may have a seepage extent that does not exceed that of the investigated areas, it is plausible that global SS emission exceeds 5 Tg yr−1

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Summary

Introduction

Methane (CH4) is a powerful greenhouse gas, whose concentrations in the atmosphere have increased about 2.5 times since the pre-industrial era (1750), approaching 1.9 ppm in 2018. Geological CH4 has erroneously been considered to be typically 13C-enriched, with relatively high δ13CCH4 values compared to biological sources such as wetlands (a global average of −38 ‰ was assumed for seepage by Sapart et al, 2012) In petroleum geochemistry it is well known, that in addition to the common thermogenic gas produced by moderate to high maturity source rocks, typically with δ13C-CH4 from −30 ‰ to about −50 ‰, vast amounts of methane in sedimentary basins are microbial ( with δ13C-CH4 ranging from −55 ‰ to about −90 ‰) and thermogenic from low maturity source rocks, with δ13CCH4 from −50 ‰ to about −70 ‰ (Etiope, 2017; Milkov and Etiope, 2018). In addition to using unrepresentatively heavy δ13C-CH4 geo-CH4 values in previous studies, detailed a priori gridded maps of geo-CH4 emissions and its isotopic signatures, which are essential for 3-D inverse modelling and for the discrimination between natural and anthropogenic microbial emissions, are currently lacking

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