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Methane is a major greenhouse gas and a key component of global biogeochemical cycles. Microbial methane often deviates from isotope and isotopolog equilibrium in surface environments but approaches equilibrium in deep subsurface sediments. The origin of this near-equilibrium isotopic signature in methane, whether directly produced by methanogens or achieved through anaerobic oxidation of methane (AOM), remains uncertain. Here, we show that, in the absence of AOM, microbial methane produced from deep-sea sediments exhibits isotopolog compositions approaching thermodynamic equilibrium due to energy limitation. In contrast, microbial methane from salt marsh and thermokarst lakes exhibits significant hydrogen and clumped isotopic disequilibrium due to high free-energy availability. We propose that clumped isotopologs of methane provide a proxy for characterizing the bioenergetics of environments for methane production. Together, these observations demonstrate methane clumped isotopes as a powerful tool to better understand the relation between methane metabolisms and the energy landscape in natural environments. 

Abstract The ongoing global temperature rise enhances permafrost thaw in the Arctic, allowing Pleistocene‐aged frozen soil organic matter to become available for microbial degradation and production of greenhouse gases, particularly methane. Here, we examined the extent and mechanism of anaerobic oxidation of methane (AOM) in the sediments of four interior Alaska thermokarst lakes, which formed and continue to expand as a result of ice‐rich permafrost thaw. In cores of surface (~ 1 m) lake sediments we quantified methane production (methanogenesis) and AOM rates using anaerobic incubation experiments in low (4°C) and high (16°C) temperatures. Methanogenesis rates were measured by the accumulation of methane over ~ 90 d, whereas AOM rates were measured by adding labeled‐¹³CH₄and measuring the produced dissolved inorganic¹³C. Our results demonstrate that while methanogenesis was vigorous in these anoxic sediments, AOM was lower by two orders of magnitude. In almost all sediment depths and temperatures, AOM rates remained less than 2% of the methanogenesis rates. Experimental evidence indicates that the AOM is strongly related to methanogens, as the addition of a methanogens' inhibitor prevented AOM. Variety of electron acceptor additions did not stimulate AOM, and methanotrophs were scarcely detected. These observations suggest that the AOM signals in the incubation experiments might be a result of enzymatic reversibility (“back‐flux”) during CH₄production, rather than thermodynamically favorable AOM. Regardless of the mechanism, the quantitative results show that near surface (< 1‐m) thermokarst sediments in interior Alaska have little to no buffer mechanisms capable of attenuating methane production in a warming climate. 

Abstract Methane (CH₄) release to the atmosphere from thawing permafrost contributes significantly to global CH₄emissions. However, constraining the effects of thaw that control the production and emission of CH₄is needed to anticipate future Arctic emissions. Here are presented robust rate measurements of CH₄production and cycling in a region of rapidly degrading permafrost. Big Trail Lake, located in central Alaska, is a young, actively expanding thermokarst lake. The lake was investigated by taking two 1 m cores of sediment from different regions. Two independent methods of measuring microbial CH₄ production, long term (CH₄accumulation) and short term (¹⁴C tracer), produced similar average rates of 11 ± 3.5 and 9 ± 3.6 nmol cm⁻³ d⁻¹, respectively. The rates had small variations between the different lithological units, indicating homogeneous CH₄production despite heterogeneous lithology in the surface ~1 m of sediment. To estimate the total CH₄production, the CH₄production rates were multiplied through the 10–15 m deep talik (thaw bulb). This estimate suggests that CH₄ production is higher than emission by a maximum factor of ~2, which is less than previous estimates. Stable and radioactive carbon isotope measurements showed that 50% of dissolved CH₄in the first meter was produced further below. Interestingly, labeled¹⁴C incubations with 2‐¹⁴C acetate and¹⁴C CO₂indicate that variations in the pathway used by microbes to produce CH₄depends on the age and type of organic matter in the sediment, but did not appear to influence the rates at which CH₄ was produced. This study demonstrates that at least half of the CH₄produced by microbial breakdown of organic matter in actively expanding thermokarst is emitted to the atmosphere, and that the majority of this CH₄is produced in the deep sediment.