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Global methane emission estimates from a dual-isotope inversion: new constraints from δD-CH4

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Methane (CH4) is a potent greenhouse gas; however, the causes of its growth since 2006 are a subject of debate. While measurements of CH4 mole fraction and carbon isotopic composition (δ13C-CH4) have been extensively used to investigate the global CH4 budget, the hydrogen isotopic composition (δD-CH4) remains underutilised despite its unique sensitivity to source types and oxidation processes. Here, we assimilate a newly harmonised 35-year dataset of dual isotope measurements from high-latitude monitoring stations in both hemispheres within a two-box Bayesian inversion to quantify global CH4 sources and sinks. The model integrates prior emissions from five source categories based on global bottom-up inventories. Methane removal processes are represented by sink-specific kinetic isotope effects as tropospheric and stratospheric loss, and soil uptake. We find that the inclusion of δD-CH4 improves the model's ability to constrain emission apportionment between biogenic and thermogenic sources, particularly for fossil fuel emissions during the late 1990s and early 2000s, which affects CH4 lifetime estimate. CH4 increase post-2006 is driven mainly by rising wetland emissions, while fossil-fuel growth is modest, biomass burning declines, and agriculture and waste make smaller, regionalised contributions. The optimised inversion results favour a strong 13C kinetic isotope effect in total tropospheric CH4 removal and a net shortening of the NH lifetime of CH4 by 0.2 years. This study demonstrates the added value of incorporating δD-CH4 into inverse modelling frameworks and underscores the importance of long-term δD-CH4 measurements for advancing our understanding of CH4 biogeochemistry and its role in the global carbon cycle.

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