Tg CH4 Yr Research Articles

Country-Scale Analysis of Methane Emissions with a High-Resolution Inverse Model Using GOSAT and Surface Observations

We employed a global high-resolution inverse model to optimize the CH4 emission using Greenhouse gas Observing Satellite (GOSAT) and surface observation data for a period from 2011–2017 for the two main source categories of anthropogenic and natural emissions. We used the Emission Database for Global Atmospheric Research (EDGAR v4.3.2) for anthropogenic methane emission and scaled them by country to match the national inventories reported to the United Nations Framework Convention on Climate Change (UNFCCC). Wetland and soil sink prior fluxes were simulated using the Vegetation Integrative Simulator of Trace gases (VISIT) model. Biomass burning prior fluxes were provided by the Global Fire Assimilation System (GFAS). We estimated a global total anthropogenic and natural methane emissions of 340.9 Tg CH4 yr−1 and 232.5 Tg CH4 yr−1, respectively. Country-scale analysis of the estimated anthropogenic emissions showed that all the top-emitting countries showed differences with their respective inventories to be within the uncertainty range of the inventories, confirming that the posterior anthropogenic emissions did not deviate from nationally reported values. Large countries, such as China, Russia, and the United States, had the mean estimated emission of 45.7 ± 8.6, 31.9 ± 7.8, and 29.8 ± 7.8 Tg CH4 yr−1, respectively. For natural wetland emissions, we estimated large emissions for Brazil (39.8 ± 12.4 Tg CH4 yr−1), the United States (25.9 ± 8.3 Tg CH4 yr−1), Russia (13.2 ± 9.3 Tg CH4 yr−1), India (12.3 ± 6.4 Tg CH4 yr−1), and Canada (12.2 ± 5.1 Tg CH4 yr−1). In both emission categories, the major emitting countries all had the model corrections to emissions within the uncertainty range of inventories. The advantages of the approach used in this study were: (1) use of high-resolution transport, useful for simulations near emission hotspots, (2) prior anthropogenic emissions adjusted to the UNFCCC reports, (3) combining surface and satellite observations, which improves the estimation of both natural and anthropogenic methane emissions over spatial scale of countries.

Methane Emission Estimates by the Global High-Resolution Inverse Model Using National Inventories

We present a global 0.1° × 0.1° high-resolution inverse model, NIES-TM-FLEXPART-VAR (NTFVAR), and a methane emission evaluation using the Greenhouse Gas Observing Satellite (GOSAT) satellite and ground-based observations from 2010–2012. Prior fluxes contained two variants of anthropogenic emissions, Emissions Database for Global Atmospheric Research (EDGAR) v4.3.2 and adjusted EDGAR v4.3.2 which were scaled to match the country totals by national reports to the United Nations Framework Convention on Climate Change (UNFCCC), augmented by biomass burning emissions from Global Fire Assimilation System (GFASv1.2) and wetlands Vegetation Integrative Simulator for Trace Gases (VISIT). The ratio of the UNFCCC-adjusted global anthropogenic emissions to EDGAR is 98%. This varies by region: 200% in Russia, 84% in China, and 62% in India. By changing prior emissions from EDGAR to UNFCCC-adjusted values, the optimized total emissions increased from 36.2 to 46 Tg CH4 yr−1 for Russia, 12.8 to 14.3 Tg CH4 yr−1 for temperate South America, and 43.2 to 44.9 Tg CH4 yr−1 for contiguous USA, and the values decrease from 54 to 51.3 Tg CH4 yr−1 for China, 26.2 to 25.5 Tg CH4 yr−1 for Europe, and by 12.4 Tg CH4 yr−1 for India. The use of the national report to scale EDGAR emissions allows more detailed statistical data and country-specific emission factors to be gathered in place compared to those available for EDGAR inventory. This serves policy needs by evaluating the national or regional emission totals reported to the UNFCCC.

Methane budget of East Asia, 1990–2015: A bottom-up evaluation

The regional budget of methane (CH4) emissions for East Asia, a crucial region in the global greenhouse gas budget, was quantified for 1990–2015 with a bottom-up method based on inventories and emission model simulations. Anthropogenic emissions associated with fossil fuel extraction, industrial activities, waste management, and agricultural activities were derived from the Emission Database for Global Atmospheric Research version 4.3.2 and compared with other inventories. Emissions from natural wetlands and CH4 uptake by upland soil oxidation were estimated using the Vegetation Integrative SImulator for Trace gases (VISIT), a biogeochemical model that considers historical land use and climatic conditions. Emissions from biomass burning and termites were calculated using satellite and land-use data combined with empirical emission factors. The resulting average annual estimated CH4 budget for 2000–2012 indicated that East Asia was a net source of 67.3 Tg CH4 yr−1, of which 88.8% was associated with anthropogenic emissions. The uncertainty (±standard deviation) of this estimate, ±14 Tg CH4 yr−1, stemmed from data and model inconsistencies. The increase of the net flux from 60.2 Tg CH4 yr−1 in 1990 to 78.0 Tg CH4 yr−1 in 2012 was due mainly to increased emissions by the fossil fuel extraction and livestock sectors. Our results showed that CH4 was a crucial component of the regional greenhouse gas budget. A spatial analysis using 0.25° × 0.25° grid cells revealed emission hotspots in urban areas, agricultural areas, and wetlands. These hotspots were surrounded by weak sinks in upland areas. The estimated natural and anthropogenic emissions fell within the range of independent estimates, including top-down estimates from atmospheric inversion models. Such a regional accounting is an effective way to elucidate climatic forcings and to develop mitigation policies. Further studies, however, are required to reduce the uncertainties in the budget.

Analysis of atmospheric CH<sub>4</sub> in Canadian Arctic and estimation of the regional CH<sub>4</sub> fluxes

Abstract. The Canadian Arctic (> 60∘ N, 60–141∘ W) may undergo drastic changes if the Arctic warming trend continues. For methane (CH4), Arctic reservoirs are large and widespread, and the climate feedbacks from such changes may be potentially substantial. Current bottom-up and top-down estimates of the regional CH4 flux range widely. This study analyzes the recent observations of atmospheric CH4 from five arctic monitoring sites and presents estimates of the regional CH4 fluxes for 2012–2015. The observational data reveal sizeable synoptic summertime enhancements in the atmospheric CH4 that are distinguishable from background variations, which indicate strong regional fluxes (primarily wetland and biomass burning CH4 emissions) around Behchoko and Inuvik in the western Canadian Arctic. Three regional Bayesian inversion modelling systems with two Lagrangian particle dispersion models and three meteorological datasets are applied to estimate fluxes for the Canadian Arctic and show relatively robust results in amplitude and temporal variations across different transport models, prior fluxes, and subregion masking. The estimated mean total CH4 flux for the entire Canadian Arctic is 1.8±0.6 Tg CH4 yr−1. The flux estimate is partitioned into biomass burning of 0.3±0.1 Tg CH4 yr−1 and the remaining natural (wetland) flux of 1.5±0.5 Tg CH4 yr−1. The summer natural CH4 flux estimates clearly show inter-annual variability that is positively correlated with surface temperature anomalies. The results indicate that years with warmer summer conditions result in more wetland CH4 emissions. More data and analysis are required to statistically characterize the dependence of regional CH4 fluxes on the climate in the Arctic. These Arctic measurement sites will aid in quantifying the inter-annual variations and long-term trends in CH4 emissions in the Canadian Arctic.

A predictive algorithm for wetlands in deep time paleoclimate models

Abstract. Methane is a powerful greenhouse gas produced in wetland environments via microbial action in anaerobic conditions. If the location and extent of wetlands are unknown, such as for the Earth many millions of years in the past, a model of wetland fraction is required in order to calculate methane emissions and thus help reduce uncertainty in the understanding of past warm greenhouse climates. Here we present an algorithm for predicting inundated wetland fraction for use in calculating wetland methane emission fluxes in deep-time paleoclimate simulations. For each grid cell in a given paleoclimate simulation, the algorithm determines the wetland fraction predicted by a nearest-neighbour search of modern-day data in a space described by a set of environmental, climate and vegetation variables. To explore this approach, we first test it for a modern-day climate with variables obtained from observations and then for an Eocene climate with variables derived from a fully coupled global climate model (HadCM3BL-M2.2; Valdes et al., 2017). Two independent dynamic vegetation models were used to provide two sets of equivalent vegetation variables which yielded two different wetland predictions. As a first test, the method, using both vegetation models, satisfactorily reproduces modern day wetland fraction at a course grid resolution, similar to those used in paleoclimate simulations. We then applied the method to an early Eocene climate, testing its outputs against the locations of Eocene coal deposits. We predict global mean monthly wetland fraction area for the early Eocene of 8×106 to 10×106 km2 with a corresponding total annual methane flux of 656 to 909 Tg CH4 yr−1, depending on which of the two different dynamic global vegetation models are used to model wetland fraction and methane emission rates. Both values are significantly higher than estimates for the modern day of 4×106 km2 and around 190 Tg CH4 yr−1 (Poulter et al., 2017; Melton et al., 2013).

China\u2019s coal mine methane regulations have not curbed growing emissions

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.

Methane budget estimates in Finland from the CarbonTracker Europe-CH4 data assimilation system

We estimated the CH4 budget in Finland for 2004–2014 using the CTE-CH4 data assimilation system with an extended atmospheric CH4 observation network of seven sites from Finland to surrounding regions (Hyytiälä, Kjølnes, Kumpula, Pallas, Puijo, Sodankylä, and Utö). The estimated average annual total emission for Finland is 0.6 ± 0.5 Tg CH4 yr−1. Sensitivity experiments show that the posterior biospheric emission estimates for Finland are between 0.3 and 0.9 Tg CH4 yr−1, which lies between the LPX-Bern-DYPTOP (0.2 Tg CH4 yr−1) and LPJG-WHyMe (2.2 Tg CH4 yr−1) process-based model estimates. For anthropogenic emissions, we found that the EDGAR v4.2 FT2010 inventory (0.4 Tg CH4 yr−1) is likely to overestimate emissions in southernmost Finland, but the extent of overestimation and possible relocation of emissions are difficult to derive from the current observation network. The posterior emission estimates were especially reliant on prior information in central Finland. However, based on analysis of posterior atmospheric CH4, we found that the anthropogenic emission distribution based on a national inventory is more reliable than the one based on EDGAR v4.2 FT2010. The contribution of total emissions in Finland to global total emissions is only about 0.13%, and the derived total emissions in Finland showed no trend during 2004–2014. The model using optimized emissions was able to reproduce observed atmospheric CH4 at the sites in Finland and surrounding regions fairly well (correlation , bias ppb), supporting adequacy of the observations to be used in atmospheric inversion studies. In addition to global budget estimates, we found that CTE-CH4 is also applicable for regional budget estimates, where small scale (11 in this case) optimization is possible with a dense observation network.

Global geological methane emissions: An update of top-down and bottom-up estimates

A wide body of literature suggests that geological gas emissions from Earth’s degassing are a major methane (CH4) source to the atmosphere. These emissions are from gas-oil seeps, mud volcanoes, microseepage and submarine seepage in sedimentary (petroleum-bearing) basins, and geothermal and volcanic manifestations. Global bottom-up emission estimates, ranging from 30 to 76 Tg CH4 yr–1, evolved in the last twenty years thanks to the increasing number of flux measurements, and improved knowledge of emission factors and area distribution (activity). Based on recent global grid maps and updated evaluations of mud volcano and microseepage emissions, the global geo-CH4 source is now (bottom-up) estimated to be 45 (27–63) Tg yr–1, i.e., ~8% of total CH4 sources. Top-down verifications, based on independent approaches (including ethane and isotopic observations) from different authors, are consistent with the range of the bottom-up estimate. However, a recent top-down study, based on radiocarbon analyses in polar ice cores, suggests that geological, fossil (14C-free) CH4 emissions about 11,600 years ago were much lower (<15 Tg yr–1, 95% CI) and that this source strength could also be valid today. Here, we show that (i) this geo-CH4 downward revision implies a fossil fuel industry CH4 upward revision of at least 24–35%. (ii) The 95% CI estimates of the recent radiocarbon analysis do not overlap with those of 5 out of 6 other bottom-up and top-down studies (no overlap for the 90% CI estimates). (iii) The contrasting lines of evidence require further discussion, and research opportunities exist to help explain this gap.

Methane emission from pan-Arctic natural wetlands estimated using a process-based model, 1901–2016

The vast pan-Arctic wetlands appear to be a large source of methane (CH4), a potent greenhouse gas. Here, I simulated CH4 emission from pan-Arctic wetlands (above 60°N) over the period 1901–2016 using a process-based biogeochemical model (VISIT), including two different schemes of wetland CH4 production, that was forced by historical atmospheric composition, climate, and land-use conditions. The two schemes simulated mean wetland CH4 emission rates of 10.9 and 11.4 Tg CH4 yr−1 in the 2000s with slightly different spatial source distributions. Both simulations showed clear seasonal cycles of CH4 emission, but the two schemes had different amplitudes and peak months. The schemes differed markedly in their simulated long-term patterns (i.e., a stationary trend and an increasing decadal trend), making it difficult to relate them to global atmospheric trends in a consistent manner. Linear regression analysis clarified the agreements and differences in environmental sensitivity and biological control of CH4 production simulated by the schemes. The time-series of CH4 emission in northern North America, northern Europe, and Siberia showed different patterns of correlation with two major meteorological teleconnection indices. This model-based study implied that the high-latitude CH4 emission accounts for 5–7% of global wetland emission and would play increasingly important roles (e.g., positive feedback) under changing climate. To reduce estimation uncertainties, as demonstrated by the comparison of two schemes, we need further studies for improving biogeochemical models in collaboration with field studies.

Bipolar carbon and hydrogen isotope constraints on the Holocene methane budget

Abstract. Atmospheric methane concentration shows a well-known decrease over the first half of the Holocene following the Northern Hemisphere summer insolation before it started to increase again to preindustrial values. There is a debate about what caused this change in the methane concentration evolution, in particular, whether an early anthropogenic influence or natural emissions led to the reversal of the atmospheric CH4 concentration evolution. Here, we present new methane concentration and stable hydrogen and carbon isotope data measured on ice core samples from both Greenland and Antarctica over the Holocene. With the help of a two-box model and the full suite of CH4 parameters, the new data allow us to quantify the total methane emissions in the Northern Hemisphere and Southern Hemisphere separately as well as their stable isotopic signatures, while interpretation of isotopic records of only one hemisphere may lead to erroneous conclusions. For the first half of the Holocene our results indicate an asynchronous decrease in Northern Hemisphere and Southern Hemisphere CH4 emissions by more than 30 Tg CH4 yr−1 in total, accompanied by a drop in the northern carbon isotopic source signature of about −3 ‰. This cannot be explained by a change in the source mix alone but requires shifts in the isotopic signature of the sources themselves caused by changes in the precursor material for the methane production. In the second half of the Holocene, global CH4 emissions increased by about 30 Tg CH4 yr−1, while preindustrial isotopic emission signatures remained more or less constant. However, our results show that this early increase in methane emissions took place in the Southern Hemisphere, while Northern Hemisphere emissions started to increase only about 2000 years ago. Accordingly, natural emissions in the southern tropics appear to be the main cause of the CH4 increase starting 5000 years before present, not supporting an early anthropogenic influence on the global methane budget by East Asian land use changes.

Advances in representing interactive methane in ModelE2-YIBs (version 1.1)

Abstract. Methane (CH4) is both a greenhouse gas and a precursor of tropospheric ozone, making it an important focus of chemistry–climate interactions. Methane has both anthropogenic and natural emission sources, and reaction with the atmosphere's principal oxidizing agent, the hydroxyl radical (OH), is the dominant tropospheric loss process of methane. The tight coupling between methane and OH abundances drives indirect linkages between methane and other short-lived air pollutants and prompts the use of interactive methane chemistry in global chemistry–climate modeling. In this study, an updated contemporary inventory of natural methane emissions and the soil sink is developed using an optimization procedure that applies published emissions data to the NASA GISS ModelE2-Yale Interactive terrestrial Biosphere (ModelE2-YIBs) global chemistry–climate model. Methane observations from the global surface air-sampling network of the Earth System Research Laboratory (ESRL) of the US National Oceanic and Atmospheric Administration (NOAA) are used to guide refinement of the natural methane inventory. The wetland methane flux is calculated as a best fit; thus, the accuracy of this derived flux assumes accurate simulation of methane chemical loss in the atmosphere and accurate prescription of the other methane fluxes (anthropogenic and natural). The optimization process indicates global annual wetland methane emissions of 140 Tg CH4 yr−1. The updated inventory includes total global annual methane emissions from natural sources of 181 Tg CH4 yr−1 and a global annual methane soil sink of 60 Tg CH4 yr−1. An interactive methane simulation is run using ModelE2-YIBs, applying dynamic methane emissions and the updated natural methane emissions inventory that results from the optimization process. The simulated methane chemical lifetime of 10.4±0.1 years corresponds well to observed lifetimes. The simulated year 2005 global-mean surface methane concentration is 1.1 % higher than the observed value from the NOAA ESRL measurements. Comparison of the simulated atmospheric methane distribution with the NOAA ESRL surface observations at 50 measurement locations finds that the simulated annual methane mixing ratio is within 1 % (i.e., +1 % to −1 %) of the observed value at 76 % of locations. Considering the 50 stations, the mean relative difference between the simulated and observed annual methane mixing ratio is a model overestimate of only 0.5 %. Comparison of simulated annual column-averaged methane concentrations with SCIAMACHY satellite retrievals provides an independent post-optimization evaluation of modeled methane. The comparison finds a slight model underestimate in 95 % of grid cells, suggesting that the applied methane source in the model is slightly underestimated or the model's methane sink strength is slightly too strong outside of the surface layer. Overall, the strong agreement between simulated and observed methane lifetimes and concentrations indicates that the ModelE2-YIBs chemistry–climate model is able to capture the principal processes that control atmospheric methane.

An assessment of natural methane fluxes simulated by the CLASS-CTEM model

Abstract. Natural methane emissions from wetlands and fire, and soil uptake of methane, simulated using the Canadian Land Surface Scheme and Canadian Terrestrial Ecosystem (CLASS-CTEM) modelling framework, over the historical 1850–2008 period, are assessed by using a one-box model of atmospheric methane burden. This one-box model also requires anthropogenic emissions and the methane sink in the atmosphere to simulate the historical evolution of global methane burden. For this purpose, global anthropogenic methane emissions for the period 1850–2008 were reconstructed based on the harmonized representative concentration pathway (RCP) and Emission Database for Global Atmospheric Research (EDGAR) data sets. The methane sink in the atmosphere is represented using bias-corrected methane lifetimes from the Canadian Middle Atmosphere Model (CMAM). The resulting evolution of atmospheric methane concentration over the historical period compares reasonably well with observation-based estimates (correlation = 0.99, root mean square error = 35 ppb). The modelled natural emissions are also assessed using an inverse procedure where the methane lifetimes required to reproduce the observed year-to-year increase in atmospheric methane burden are calculated based upon the specified global anthropogenic and modelled natural emissions that we have used here. These calculated methane lifetimes over the historical period fall within the uncertainty range of observation-based estimates. The present-day (2000–2008) values of modelled methane emissions from wetlands (169 Tg CH4 yr−1) and fire (27 Tg CH4 yr−1), methane uptake by soil (29 Tg CH4 yr−1), and the budget terms associated with overall anthropogenic and natural emissions are consistent with estimates reported in a recent global methane budget that is based on top-down approaches constrained by observed atmospheric methane burden. The modelled wetland emissions increase over the historical period in response to both increases in precipitation and in atmospheric CO2 concentration. This increase in wetland emissions over the historical period yields evolution of the atmospheric methane concentration that compares better with observation-based values than the case when wetland emissions are held constant over the historical period.

Enhanced response of global wetland methane emissions to the 2015–2016 El Niño-Southern Oscillation event

Wetlands are thought to be the major contributor to interannual variability in the growth rate of atmospheric methane (CH4) with anomalies driven by the influence of the El Niño-Southern Oscillation (ENSO). Yet it remains unclear whether (i) the increase in total global CH4 emissions during El Niño versus La Niña events is from wetlands and (ii) how large the contribution of wetland CH4 emissions is to the interannual variability of atmospheric CH4. We used a terrestrial ecosystem model that includes permafrost and wetland dynamics to estimate CH4 emissions, forced by three separate meteorological reanalyses and one gridded observational climate dataset, to simulate the spatio-temporal dynamics of wetland CH4 emissions from 1980–2016. The simulations show that while wetland CH4 responds with negative annual anomalies during the El Niño events, the instantaneous growth rate of wetland CH4 emissions exhibits complex phase dynamics. We find that wetland CH4 instantaneous growth rates were declined at the onset of the 2015–2016 El Niño event but then increased to a record-high at later stages of the El Niño event (January through May 2016). We also find evidence for a step increase of CH4 emissions by 7.8±1.6 Tg CH4 yr−1 during 2007–2014 compared to the average of 2000–2006 from simulations using meteorological reanalyses, which is equivalent to a ~3.5 ppb yr−1 rise in CH4 concentrations. The step increase is mainly caused by the expansion of wetland area in the tropics (30°S–30°N) due to an enhancement of tropical precipitation as indicated by the suite of the meteorological reanalyses. Our study highlights the role of wetlands, and the complex temporal phasing with ENSO, in driving the variability and trends of atmospheric CH4 concentrations. In addition, the need to account for uncertainty in meteorological forcings is highlighted in addressing the interannual variability and decadal-scale trends of wetland CH4 fluxes.

Soil Methanotrophy Model (MeMo v1.0): a process-based model to quantify global uptake of atmospheric methane by soil

Abstract. Soil bacteria known as methanotrophs are the sole biological sink for atmospheric methane (CH4), a potent greenhouse gas that is responsible for ∼ 20 % of the human-driven increase in radiative forcing since pre-industrial times. Soil methanotrophy is controlled by a plethora of factors, including temperature, soil texture, moisture and nitrogen content, resulting in spatially and temporally heterogeneous rates of soil methanotrophy. As a consequence, the exact magnitude of the global soil sink, as well as its temporal and spatial variability, remains poorly constrained. We developed a process-based model (Methanotrophy Model; MeMo v1.0) to simulate and quantify the uptake of atmospheric CH4 by soils at the global scale. MeMo builds on previous models by Ridgwell et al. (1999) and Curry (2007) by introducing several advances, including (1) a general analytical solution of the one-dimensional diffusion–reaction equation in porous media, (2) a refined representation of nitrogen inhibition on soil methanotrophy, (3) updated factors governing the influence of soil moisture and temperature on CH4 oxidation rates and (4) the ability to evaluate the impact of autochthonous soil CH4 sources on uptake of atmospheric CH4. We show that the improved structural and parametric representation of key drivers of soil methanotrophy in MeMo results in a better fit to observational data. A global simulation of soil methanotrophy for the period 1990–2009 using MeMo yielded an average annual sink of 33.5 ± 0.6 Tg CH4 yr−1. Warm and semi-arid regions (tropical deciduous forest and open shrubland) had the highest CH4 uptake rates of 602 and 518 mg CH4 m−2 yr−1, respectively. In these regions, favourable annual soil moisture content (∼ 20 % saturation) and low seasonal temperature variations (variations < ∼ 6 ∘C) provided optimal conditions for soil methanotrophy and soil–atmosphere gas exchange. In contrast to previous model analyses, but in agreement with recent observational data, MeMo predicted low fluxes in wet tropical regions because of refinements in formulation of the influence of excess soil moisture on methanotrophy. Tundra and mixed forest had the lowest simulated CH4 uptake rates of 176 and 182 mg CH4 m−2 yr−1, respectively, due to their marked seasonality driven by temperature. Global soil uptake of atmospheric CH4 was decreased by 4 % by the effect of nitrogen inputs to the system; however, the direct addition of fertilizers attenuated the flux by 72 % in regions with high agricultural intensity (i.e. China, India and Europe) and by 4–10 % in agriculture areas receiving low rates of N input (e.g. South America). Globally, nitrogen inputs reduced soil uptake of atmospheric CH4 by 1.38 Tg yr−1, which is 2–5 times smaller than reported previously. In addition to improved characterization of the contemporary soil sink for atmospheric CH4, MeMo provides an opportunity to quantify more accurately the relative importance of soil methanotrophy in the global CH4 cycle in the past and its capacity to contribute to reduction of atmospheric CH4 levels under future global change scenarios.

Large methane emissions from natural gas vehicles in Chinese cities

In recent years, cities in developing countries have become more and more reliant on natural gas as a clean energy source for transportation to reduce air pollution. In this study, we used street-level measurement of atmospheric CH4 and CO2 concentrations to quantify CH4 emissions from natural gas vehicles (NGVs) in China. These measurements were made in eight cities (Chengdu, Urumqi, Jinan, Nanjing, Lanzhou, Harbin, Guangzhou) with varying sizes of NGV fleet. A traffic CH4:CO2 emission ratio (TER) was determined via linear regression of CH4 versus CO2 concentration data obtained from each street transect. The TER value was combined with the ratio of NGVs in the street traffic in a mathematical model to obtain the CH4 emission factor for NGVs. Results show that the TER increases with increasing NGV ratio and decreases with increasing traffic speed. Overall, the NGV CH4 emission factor in these cities is 0.022 ± 0.0033 kg m−3, about 8 times the Intergovernmental Panel on Climate Change (IPCC) default factor for NGVs and is more than 100% higher than the mean NGV tailpipe emission factor found in the published literature. That the overall emission factor is much larger than the tailpipe emission factor indicates that on-road vehicle gas leakage is a widespread problem. A business-as-usual scenario suggests that NGVs may emit 1.23 Tg CH4 yr−1 in 2030, or about 3% of China's current total anthropogenic emission. Our study suggest that curbing the emissions from this sector should be a high priority for global climate mitigation efforts.

Quantification of methane sources in the Athabasca Oil Sands Region of Alberta by aircraft mass balance

Abstract. Aircraft-based measurements of methane (CH4) and other air pollutants in the Athabasca Oil Sands Region (AOSR) were made during a summer intensive field campaign between 13 August and 7 September 2013 in support of the Joint Canada–Alberta Implementation Plan for Oil Sands Monitoring. Chemical signatures were used to identify CH4 sources from tailings ponds (BTEX VOCs), open pit surface mines (NOy and rBC) and elevated plumes from bitumen upgrading facilities (SO2 and NOy). Emission rates of CH4 were determined for the five primary surface mining facilities in the region using two mass-balance methods. Emission rates from source categories within each facility were estimated when plumes from the sources were spatially separable. Tailings ponds accounted for 45 % of total CH4 emissions measured from the major surface mining facilities in the region, while emissions from operations in the open pit mines accounted for ∼ 50 %. The average open pit surface mining emission rates ranged from 1.2 to 2.8 t of CH4 h−1 for different facilities in the AOSR. Amongst the 19 tailings ponds, Mildred Lake Settling Basin, the oldest pond in the region, was found to be responsible for the majority of tailings ponds emissions of CH4 (> 70 %). The sum of measured emission rates of CH4 from the five major facilities, 19.2 ± 1.1 t CH4 h−1, was similar to a single mass-balance determination of CH4 from all major sources in the AOSR determined from a single flight downwind of the facilities, 23.7 ± 3.7 t CH4 h−1. The measured hourly CH4 emission rate from all facilities in the AOSR is 48 ± 8 % higher than that extracted for 2013 from the Canadian Greenhouse Gas Reporting Program, a legislated facility-reported emissions inventory, converted to hourly units. The measured emissions correspond to an emissions rate of 0.17 ± 0.01 Tg CH4 yr−1 if the emissions are assumed as temporally constant, which is an uncertain assumption. The emission rates reported here are relevant for the summer season. In the future, effort should be devoted to measurements in different seasons to further our understanding of the seasonal parameters impacting fugitive emissions of CH4 and to allow for better estimates of annual emissions and year-to-year variability.

Temporal Variations of the Mole Fraction, Carbon, and Hydrogen Isotope Ratios of Atmospheric Methane in the Hudson Bay Lowlands, Canada

AbstractWe have conducted simultaneous measurements of the mole fraction and carbon and hydrogen isotope ratios (δ13C and δD) of atmospheric methane (CH4) at Churchill (58°44′N, 93°49′W) in the northern part of the Hudson Bay Lowlands (HBL), Canada, since 2007. Compared with the measurements at an Arctic baseline monitoring station, Ny‐Ålesund, Svalbard (78°55′N, 11°56′E), CH4 mole fraction is generally higher and δ13C and δD are lower at Churchill due to regional biogenic CH4 emissions. Clear seasonal cycles in the CH4 mole fraction, δ13C, and δD are observable at Churchill, and their seasonal phases in summer are earlier by approximately 2 weeks than those at Ny‐Ålesund. Using the one‐box model analysis, the phase difference is ascribed to the different seasonal influence of CH4 emissions from boreal wetlands on the two sites. Short‐term CH4 variations are also observed at Churchill throughout the year. The analysis of the observed isotopic signatures of atmospheric CH4 confirmed that the short‐term CH4 variations are mainly produced by biogenic CH4 released from the HBL wetlands in summer and by fossil fuel CH4 transported over the Arctic in winter. Forward simulations of an atmospheric chemistry‐transport model, with wetland CH4 fluxes prescribed by a process‐based model, show unrealistically high CH4 mole fractions at Churchill in summer, suggesting that CH4 emissions assigned to the HBL wetlands are overestimated. Our best estimate of the HBL CH4 emissions is 2.7 ± 0.3 Tg CH4 yr−1 as an average of 2007–2013, consistent with recent estimations by inverse modeling studies.

Inventory of methane emissions from livestock in China from 1980 to 2013

Livestock is the largest anthropogenic methane (CH4) source at the global scale. Previous inventories of this source for China were based on the accounting of livestock populations and constant emission factors (EFs) per head. Here, we re-evaluate how livestock CH4 emissions have changed from China over the last three decades, considering increasing population, body weight and milk production per head which cause EF to change with time, and decreasing average life span (ALS) of livestock. Our results show that annual CH4 emissions by livestock have increased from 4.5 to 11.8 Tg CH4 yr−1 over the period 1980–2013. The increasing trend in emissions (0.25 Tg CH4 yr−2) over this period is ∼12% larger than that if using constant EFs and ALS. The increasing livestock population, production per head and decreasing ALS contributed +91%, +28% and −19% to the increase in CH4 emissions from livestock, respectively. This implies that the temporal changes in EF and ALS of livestock cannot be overlooked in inventories, especially in countries like China where livestock production systems are experiencing rapid transformations.

Dissolved methane in the East China Sea: Distribution, seasonal variation and emission

We present a dataset of dissolved methane (CH4) in the East China Sea (ECS) during five cruises in March, May, August, October and December 2011. CH4 distribution in this region showed pronounced spatial and seasonal variability due to the complex mixing of different water masses and other variables. Surface CH4 concentrations gradually decreased from the coast to the open sea, with maximum values occurring near Changjiang estuary or outside the Hangzhou Bay. The annual mean CH4 concentration of the surface layer was 9.1 ± 1.6 nmol L-1 in the coastal area, which was nearly twice as large as that in the open sea (4.3 ± 1.3 nmol L-1). CH4 was distributed evenly from the surface to the bottom in the shelf region during March and December, while it increased gradually with depth during May and October. CH4 depth profiles exhibited various distribution features along the coast, in the middle and on the edge of continental shelf. CH4 levels at the bottom were generally higher than at the surface during all seasons, indicating obvious CH4 sources from sediments. Incubation experiments of sediment cores onboard suggested that sediment release was an important source of CH4 in the water column of the ECS. We estimated that the annual average CH4 release rate from sediments was about 1.11 μmol·m-2·d-1 on the continental shelf of the ECS. The maximum CH4 concentration and sediment-water CH4 flux both occurred in summer, which might be related with the occurrence of hypoxia in the bottom water. Surface seawater of the ECS was oversaturated with CH4 relative to the atmosphere over most of the five cruises, indicating that the ECS was a net source of atmospheric CH4. The annual mean area-weighted sea-air flux density of CH4 in the ECS was estimated to be about 10.7 μmol·m-2·d-1 in 2011. Accordingly, an area-weighted, seasonally adjusted annual rate of CH4 efflux was determined to be 2.98 × 109 mol yr-1 (∼0.05 Tg CH4 yr-1) from the ECS to the atmosphere.

Source Partitioning of Methane Emissions and its Seasonality in the U.S. Midwest.

The methane (CH4) budget and its source partitioning are poorly constrained in the Midwestern United States. We used tall tower (185 m) aerodynamic flux measurements and atmospheric scale factor Bayesian inversions to constrain the monthly budget and to partition the total budget into natural (e.g., wetlands) and anthropogenic (e.g., livestock, waste, and natural gas) sources for the period June 2016 to September 2017. Aerodynamic flux observations indicated that the landscape was a CH4 source with a mean annual CH4 flux of +13.7 ± 0.34 nmol m-2 s-1 and was rarely a net sink. The scale factor Bayesian inversion analyses revealed a mean annual source of +12.3 ± 2.1 nmol m-2 s-1. Flux partitioning revealed that the anthropogenic source (7.8 ± 1.6 Tg CH4 yr-1) was 1.5 times greater than the bottom-up gridded United States Environmental Protection Agency inventory, in which livestock and oil/gas sources were underestimated by 1.8-fold and 1.3-fold, respectively. Wetland emissions (4.0 ± 1.2 Tg CH4 yr-1) were the second largest source, accounting for 34% of the total budget. The temporal variability of total CH4 emissions was dominated by wetlands with peak emissions occurring in August. In contrast, emissions from oil/gas and other anthropogenic sources showed relatively weak seasonality.