Methane has the second-largest global radiative forcing impact of anthropogenic greenhouse gases after carbon dioxide, but our understanding of the global atmospheric methane budget is incomplete. The global fossil fuel industry (production and usage of natural gas, oil and coal) is thought to contribute 15 to 22 per cent of methane emissions to the total atmospheric methane budget. However, questions remain regarding methane emission trends as a result of fossil fuel industrial activity and the contribution to total methane emissions of sources from the fossil fuel industry and from natural geological seepage, which are often co-located. Here we re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions based on long-term global methane and methane carbon isotope records. We compile the largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources. We find that total fossil fuel methane emissions (fossil fuel industry plus natural geological seepage) are not increasing over time, but are 60 to 110 per cent greater than current estimates owing to large revisions in isotope source signatures. We show that this is consistent with the observed global latitudinal methane gradient. After accounting for natural geological methane seepage, we find that methane emissions from natural gas, oil and coal production and their usage are 20 to 60 per cent greater than inventories. Our findings imply a greater potential for the fossil fuel industry to mitigate anthropogenic climate forcing, but we also find that methane emissions from natural gas as a fraction of production have declined from approximately 8 per cent to approximately 2 per cent over the past three decades.

Abstract. The concentration of atmospheric methane (CH 4 ) has more than doubled over the industrial era. To help constrain global and regional CH 4 budgets, inverse (top-down) models incorporate data on the concentration and stable carbon (δ 13 C) and hydrogen (δ 2 H) isotopic ratios of atmospheric CH 4 . These models depend on accurate δ 13 C and δ 2 H end-member source signatures for each of the main emissions categories. Compared with meticulous measurement and calibration of isotopic CH 4 in the atmosphere, there has been relatively less effort to characterize globally representative isotopic source signatures, particularly for fossil fuel sources. Most global CH 4 budget models have so far relied on outdated source signature values derived from globally nonrepresentative data. To correct this deficiency, we present a comprehensive, globally representative end-member database of the δ 13 C and δ 2 H of CH 4 from fossil fuel (conventional natural gas, shale gas, and coal), modern microbial (wetlands, rice paddies, ruminants, termites, and landfills and/or waste) and biomass burning sources. Gas molecular compositional data for fossil fuel categories are also included with the database. The database comprises 10 706 samples (8734 fossil fuel, 1972 non-fossil) from 190 published references. Mean (unweighted) δ 13 C signatures for fossil fuel CH 4 are significantly lighter than values commonly used in CH 4 budget models, thus highlighting potential underestimation of fossil fuel CH 4 emissions in previous CH 4 budget models. This living database will be updated every 2-3 years to provide the atmospheric modeling community with the most complete CH 4 source signature data possible. Database digital object identifier (DOI): https://doi.org/10.15138/G3201T.

Anthropogenic methane emissions from China are likely greater than in any other country in the world. The largest fraction of China’s anthropogenic emissions is attributable to coal mining, but these emissions may be changing; China enacted a suite of regulations for coal mine methane (CMM) drainage and utilization that came into full effect in 2010. Here, we use methane observations from the GOSAT satellite to evaluate recent trends in total anthropogenic and natural emissions from Asia with a particular focus on China. We find that emissions from China rose by 1.1 ± 0.4 Tg CH4 yr−1 from 2010 to 2015, culminating in total anthropogenic and natural emissions of 61.5 ± 2.7 Tg CH4 in 2015. The observed trend is consistent with pre-2010 trends and is largely attributable to coal mining. These results indicate that China’s CMM regulations have had no discernible impact on the continued increase in Chinese methane emissions.

Abstract. Airborne estimates of greenhouse gas emissions are becoming more prevalent with the advent of rapid commercial development of trace gas instrumentation featuring increased measurement accuracy, precision, and frequency, and the swelling interest in the verification of current emission inventories. Multiple airborne studies have indicated that emission inventories may underestimate some hydrocarbon emission sources in US oil-and gas-producing basins. Consequently, a proper assessment of the accuracy of these airborne methods is crucial to interpreting the meaning of such discrepancies. We present a new method of sampling surface sources of any trace gas for which fast and precise measurements can be made and apply it to methane, ethane, and carbon dioxide on spatial scales of ∼ 1000 m, where consecutive loops are flown around a targeted source region at multiple altitudes. Using Reynolds decomposition for the scalar concentrations, along with Gauss's theorem, we show that the method accurately accounts for the smallerscale turbulent dispersion of the local plume, which is often ignored in other average "mass balance" methods. With the help of large eddy simulations (LES) we further show how the circling radius can be optimized for the micrometeorological conditions encountered during any flight. Furthermore, by sampling controlled releases of methane and ethane on the ground we can ascertain that the accuracy of the method, in appropriate meteorological conditions, is often better than 10 %, with limits of detection below 5 kg h −1 for both methane and ethane. Because of the FAA-mandated minimum flight safe altitude of 150 m, placement of the aircraft is critical to preventing a large portion of the emission plume from flowing underneath the lowest aircraft sampling altitude, which is generally the leading source of uncertainty in these measurements. Finally, we show how the accuracy of the method is strongly dependent on the number of sampling loops and/or time spent sampling the source plume.

Airborne measurements of methane emissions from oil and gas infrastructure were completed over two regions of Alberta, Canada. These top-down measurements were directly compared with region-specific bottom-up inventories that utilized current industry-reported flaring and venting volumes (reported data) and quantitative estimates of unreported venting and fugitive sources. For the 50 × 50 km measurement region near Red Deer, characterized by natural gas and light oil production, measured methane fluxes were more than 17 times greater than that derived from directly reported data but consistent with our region-specific bottom-up inventory-based estimate. For the 60 × 60 km measurement region near Lloydminster, characterized by significant cold heavy oil production with sand (CHOPS), airborne measured methane fluxes were five times greater than directly reported emissions from venting and flaring and four times greater than our region-specific bottom up inventory-based estimate. Extended across Alberta, our results suggest that reported venting emissions in Alberta should be 2.5 ± 0.5 times higher, and total methane emissions from the upstream oil and gas sector (excluding mined oil sands) are likely at least 25-50% greater than current government estimates. Successful mitigation efforts in the Red Deer region will need to focus on the >90% of methane emissions currently unmeasured or unreported.

Divergence in recent oil and gas related methane emission estimates between aircraft studies (basin total for a midday window) and emissions inventories (annualized regional and national statistics) indicate the need for better understanding the experimental design, including temporal and spatial alignment and interpretation of results. Our aircraft-based methane emission estimates in a major U.S. shale gas basin resolved from west to east show (i) similar spatial distributions for 2 days, (ii) strong spatial correlations with reported NG production (R = 0.75) and active gas well pad count (R = 0.81), and (iii) 2× higher emissions in the western half (normalized by gas production) despite relatively homogeneous dry gas and well characteristics. Operator reported hourly activity data show that midday episodic emissions from manual liquid unloadings (a routine operation in this basin and elsewhere) could explain ∼1/3 of the total emissions detected midday by the aircraft and ∼2/3 of the west-east difference in emissions. The 22% emission difference between both days further emphasizes that episodic sources can substantially impact midday methane emissions and that aircraft may detect daily peak emissions rather than daily averages that are generally employed in emissions inventories. While the aircraft approach is valid, quantitative, and independent, our study sheds new light on the interpretation of previous basin scale aircraft studies, and provides an improved mechanistic understanding of oil and gas related methane emissions.

SignificanceOur results demonstrate that access to high-resolution spatiotemporal activity data and multiscale, contemporaneous measurements is critical to understanding oil- and gas-related methane emissions. Careful consideration of all factors influencing methane emissions—including temporal variation—is necessary in scientific and policy discussions to develop effective strategies for mitigating greenhouse gas emissions from natural gas infrastructure.

The amount of methane emissions released by the natural gas (NG) industry is a critical and uncertain value for various industry and policy decisions, such as for determining the climate implications of using NG over coal. Previous studies have estimated fugitive emissions rates (FER)--the fraction of produced NG (mainly methane and ethane) escaped to the atmosphere--between 1 and 9%. Most of these studies rely on few and outdated measurements, and some may represent only temporal/regional NG industry snapshots. This study estimates NG industry representative FER using global atmospheric methane and ethane measurements over three decades, and literature ranges of (i) tracer gas atmospheric lifetimes, (ii) non-NG source estimates, and (iii) fossil fuel fugitive gas hydrocarbon compositions. The modeling suggests an upper bound global average FER of 5% during 2006-2011, and a most likely FER of 2-4% since 2000, trending downward. These results do not account for highly uncertain natural hydrocarbon seepage, which could lower the FER. Further emissions reductions by the NG industry may be needed to ensure climate benefits over coal during the next few decades.