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Abstract Dissolved gas concentrations in surface waters can have sharp gradients across marine and freshwater environments, which often prove challenging to capture with analytical measurement. Collecting discrete samples for laboratory analysis provides accurate results, but suffers from poor spatial resolution. To overcome this limitation, water equilibrators and gas membrane contactors (GMCs) have been used for the automated underway measurement of dissolved gas concentrations in surface water. However, while water equilibrators can provide continuous measurements, their analytical response times to changes in surface water concentration can be slow, lasting tens of minutes. This leads to spatial imprecisions in the dissolved gas concentration data. Conversely, while GMCs have proven to have much faster analytical response times, often lasting only a few minutes or less, they suffer from poor accuracy and thus require routine calibration. Here we present an analytical system for the high accuracy and high precision spatial mapping of dissolved methane concentration in surface waters. The system integrates a GMC with a cavity ringdown spectrometer for fast analytical response times, with a calibration method involving two Weiss‐style equilibrators and discrete measurements in vials. Data from both the GMC and equilibrators are collected simultaneously, with discrete vial samples collected periodically throughout data collection. We also present a mathematical algorithm integrating all data collected for the routine calibration of the GMC dataset. The algorithm facilitates comparison between the GMC and equilibrator datasets despite the substantial differences in response times (0.7–2.1 and 4.1–17.6 min, respectively). This measurement system was tested with both systematic laboratory experiments and field data collected on a research cruise along the US Atlantic margin. Once calibrated, this system identified numerous sharp peaks of dissolved methane concentration in the US Atlantic margin dataset that would be poorly resolved, or outright missed with previous measurement techniques. Overall, the precision and accuracy for the technique presented here were determined to be 11.2% and 10.4%, respectively, the operating range was 0–1000 ppm methane, and thee‐folding response time to changes in dissolved methane concentration was 0.7–2.1 min. 

Abstract The coastal ocean contributes to regulating atmospheric greenhouse gas concentrations by taking up carbon dioxide (CO₂) and releasing nitrous oxide (N₂O) and methane (CH₄). In this second phase of the Regional Carbon Cycle Assessment and Processes (RECCAP2), we quantify global coastal ocean fluxes of CO₂, N₂O and CH₄using an ensemble of global gap‐filled observation‐based products and ocean biogeochemical models. The global coastal ocean is a net sink of CO₂in both observational products and models, but the magnitude of the median net global coastal uptake is ∼60% larger in models (−0.72 vs. −0.44 PgC year⁻¹, 1998–2018, coastal ocean extending to 300 km offshore or 1,000 m isobath with area of 77 million km²). We attribute most of this model‐product difference to the seasonality in sea surface CO₂partial pressure at mid‐ and high‐latitudes, where models simulate stronger winter CO₂uptake. The coastal ocean CO₂sink has increased in the past decades but the available time‐resolving observation‐based products and models show large discrepancies in the magnitude of this increase. The global coastal ocean is a major source of N₂O (+0.70 PgCO₂‐e year⁻¹in observational product and +0.54 PgCO₂‐e year⁻¹in model median) and CH₄(+0.21 PgCO₂‐e year⁻¹in observational product), which offsets a substantial proportion of the coastal CO₂uptake in the net radiative balance (30%–60% in CO₂‐equivalents), highlighting the importance of considering the three greenhouse gases when examining the influence of the coastal ocean on climate. 

Abstract Geological sources of methane (CH₄), such as hydrocarbon seeps, are significant yet poorly constrained sources of CH₄to seawater and the overlying atmosphere_.We investigate the radiocarbon content (¹⁴C) and concentrations of dissolved CH₄in surface waters from the Coal Oil Point seep field to test the hypothesis that geological sources can dominate the regional background signal of CH₄. We find that surface waters with elevated CH₄concentration were populated with seep‐CH₄and that lower concentrations of CH₄were well explained by mixing with the regional background of nongeological CH₄. Substantial differences in concentration and¹⁴C‐CH₄were observed over distances <5 km, demonstrating that surface currents mix background‐CH₄into the seep field. These results indicate that even a prolific seep region like the Santa Barbara Basin exerts limited influence on the regional background of CH₄in the surface layer but is a significant driver of patchiness in oceanic CH₄biogeochemistry. 

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Emissions and atmospheric concentrations of CH4 continue to increase, maintaining CH4 as 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 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the factors explaining the well-observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in-situ and greenhouse gas observing satellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land-surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full datasets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this edition benefits from important progress in estimating inland freshwater emissions, with better accounting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double accounting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double accounting that still exists (average of 23 Tg CH4 yr-1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr-1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr-1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr-1 or ~65 % are attributed to direct anthropogenic sources in the fossil, agriculture and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr-1 or 63–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr-1 (range 9–40). Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr-1) larger global emissions (669 Tg CH4 yr-1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr-1 in Saunois et al. (2016, 2020), respectively), and for the first time uncertainty in bottom-up and top-down budgets overlap. The latitudinal distribution from atmospheric inversion-based emissions indicates a predominance of tropical and southern hemisphere emissions (~65 % of the global budget, <30° N) compared to mid (30° N–60° N, ~30 % of emissions) and high-northern latitudes (60° N–90° N, ~4 % of global emissions). This latitudinal distribution is similar in the bottom-up budget though the bottom-up budget estimates slightly larger contributions for the mid and high-northern latitudes, and slightly smaller contributions from the tropics and southern hemisphere than the inversions. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. We identify five major priorities for improving the CH4 budget: i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; ii) further development of process-based models for inland-water emissions; iii) intensification of CH4 observations at local (e.g., FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; iv) improvements of transport models and the representation of photochemical sinks in top-down inversions, and v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024). 

During investigations of aerobic methane oxidation, this study found that seafloor seeps emit low pH water alongside methane. This discovery was revealed through isotopic measurement and model experiments. 

Abstract. In the current era of rapid climate change, accuratecharacterization of climate-relevant gas dynamics – namely production,consumption, and net emissions – is required for all biomes, especially thoseecosystems most susceptible to the impact of change. Marine environmentsinclude regions that act as net sources or sinks for numerous climate-activetrace gases including methane (CH4) and nitrous oxide (N2O). Thetemporal and spatial distributions of CH4 and N2O are controlledby the interaction of complex biogeochemical and physical processes. Toevaluate and quantify how these mechanisms affect marine CH4 andN2O cycling requires a combination of traditional scientificdisciplines including oceanography, microbiology, and numerical modeling.Fundamental to these efforts is ensuring that the datasets produced byindependent scientists are comparable and interoperable. Equally critical istransparent communication within the research community about the technicalimprovements required to increase our collective understanding of marineCH4 and N2O. A workshop sponsored by Ocean Carbon and Biogeochemistry (OCB)was organized to enhance dialogue and collaborations pertaining tomarine CH4 and N2O. Here, we summarize the outcomes from theworkshop to describe the challenges and opportunities for near-futureCH4 and N2O research in the marine environment. 

Abstract. Understanding and quantifying the global methane (CH4) budgetis 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 interms of climate forcing, after carbon dioxide (CO2). The relativeimportance of CH4 compared to CO2 depends on its shorteratmospheric lifetime, stronger warming potential, and variations inatmospheric growth rate over the past decade, the causes of which are stilldebated. Two major challenges in reducing uncertainties in the atmosphericgrowth rate arise from the variety of geographically overlapping CH4sources and from the destruction of CH4 by short-lived hydroxylradicals (OH). To address these challenges, we have established aconsortium of multidisciplinary scientists under the umbrella of the GlobalCarbon Project to synthesize and stimulate new research aimed at improvingand regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paperdedicated to the decadal methane budget, integrating results of top-downstudies (atmospheric observations within an atmospheric inverse-modellingframework) and bottom-up estimates (including process-based models forestimating land surface emissions and atmospheric chemistry, inventories ofanthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated byatmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximumestimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or∼ 60 % is attributed to anthropogenic sources, that isemissions 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) is29 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 previousbudget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4emissions have been tracking the warmest scenarios assessed by theIntergovernmental Panel on Climate Change. Bottom-up methods suggest almost30 % larger global emissions (737 Tg CH4 yr−1, range 594–881)than top-down inversion methods. Indeed, bottom-up estimates for naturalsources such as natural wetlands, other inland water systems, and geologicalsources are higher than top-down estimates. The atmospheric constraints onthe top-down budget suggest that at least some of these bottom-up emissionsare overestimated. The latitudinal distribution of atmosphericobservation-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 methanebudget is attributable to natural emissions, especially those from wetlandsand other inland waters. Some of our global source estimates are smaller than those in previouslypublished budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due toimproved partition wetlands and other inland waters. Emissions fromgeological 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 overalldiscrepancy between bottom-up and top-down estimates has been reduced byonly 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 methanebudget include (i) a global, high-resolution map of water-saturated soilsand inundated areas emitting methane based on a robust classification ofdifferent types of emitting habitats; (ii) further development ofprocess-based models for inland-water emissions; (iii) intensification ofmethane observations at local scales (e.g., FLUXNET-CH4 measurements)and urban-scale monitoring to constrain bottom-up land surface models, andat regional scales (surface networks and satellites) to constrainatmospheric inversions; (iv) improvements of transport models and therepresentation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/orco-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded fromhttps://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from theGlobal Carbon Project.