Geographic variability in freshwater methane hydrogen isotope ratios and its implications for global isotopic source signatures

Abstract. There is growing interest in developing spatially resolved methane (CH4) isotopic source signatures to aid in geographic source attribution of CH4 emissions. CH4 hydrogen isotope measurements (δ2H–CH4) have the potential to be a powerful tool for geographic differentiation of CH4 emissions from freshwater environments, as well as other microbial sources. This is because microbial δ2H–CH4 values are partially dependent on the δ2H of environmental water (δ2H–H2O), which exhibits large and well-characterized spatial variability globally. We have refined the existing global relationship between δ2H–CH4 and δ2H–H2O by compiling a more extensive global dataset of δ2H–CH4 from freshwater environments, including wetlands, inland waters, and rice paddies, comprising a total of 129 different sites, and compared these with measurements and estimates of δ2H–H2O, as well as δ13C-CH4 and δ13C–CO2 measurements. We found that estimates of δ2H–H2O explain approximately 42 % of the observed variation in δ2H–CH4, with a flatter slope than observed in previous studies. The inferred global δ2H–CH4 vs. δ2H–H2O regression relationship is not sensitive to using either modelled precipitation δ2H or measured δ2H–H2O as the predictor variable. The slope of the global freshwater relationship between δ2H–CH4 and δ2H–H2O is similar to observations from incubation experiments but is different from pure culture experiments. This result is consistent with previous suggestions that variation in the δ2H of acetate, controlled by environmental δ2H–H2O, is important in determining variation in δ2H–CH4. The relationship between δ2H–CH4 and δ2H–H2O leads to significant differences in the distribution of freshwater δ2H–CH4 between the northern high latitudes (60–90∘ N), relative to other global regions. We estimate a flux-weighted global freshwater δ2H–CH4 of −310 ± 15 ‰, which is higher than most previous estimates. Comparison with δ13C measurements of both CH4 and CO2 implies that residual δ2H–CH4 variation is the result of complex interactions between CH4 oxidation, variation in the dominant pathway of methanogenesis, and potentially other biogeochemical variables. We observe a significantly greater distribution of δ2H–CH4 values, corrected for δ2H–H2O, in inland waters relative to wetlands, and suggest this difference is caused by more prevalent CH4 oxidation in inland waters. We used the expanded freshwater CH4 isotopic dataset to calculate a bottom-up estimate of global source δ2H–CH4 and δ13C-CH4 that includes spatially resolved isotopic signatures for freshwater CH4 sources. Our bottom-up global source δ2H–CH4 estimate (−278 ± 15 ‰) is higher than a previous estimate using a similar approach, as a result of the more enriched global freshwater δ2H–CH4 signature derived from our dataset. However, it is in agreement with top-down estimates of global source δ2H–CH4 based on atmospheric measurements and estimated atmospheric sink fractionations. In contrast our bottom-up global source δ13C-CH4 estimate is lower than top-down estimates, partly as a result of a lack of δ13C-CH4 data from C4-plant-dominated ecosystems. In general, we find there is a particular need for more data to constrain isotopic signatures for low-latitude microbial CH4 sources.

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Global geographic variability in freshwater methane hydrogen isotope ratios and its implications for emissions source apportionment and microbial biogeochemistry

10.5194/bg-2020-410 ◽

2020 ◽

Author(s):

Peter M. J. Douglas ◽

Emerald Stratigopoulos ◽

Jenny Park ◽

Dawson Phan

Keyword(s):

Hydrogen Isotope ◽

Environmental Water ◽

Freshwater Ecosystems ◽

Rice Paddies ◽

Source Attribution ◽

Atmospheric Measurements ◽

Ch4 Emissions ◽

Spatially Resolved ◽

Hydrogenotrophic Methanogenesis ◽

Freshwater Environments

Abstract. There is growing interest in developing spatially resolved methane (CH4) isotopic source signatures to aid in geographic source attribution of CH4 emissions. CH4 hydrogen isotope measurements (δ2H-CH4) have the potential to be a powerful tool for spatial resolution of CH4 emissions from freshwater environments, as well as other microbial sources. This is because microbial δ2H-CH4 values are partially dependent on the δ2H of environmental water (δ2H-H2O), which exhibits large and well-characterized spatial variability globally. We compiled a comprehensive global dataset of paired CH4 δ2H and δ13C measurements from freshwater environments, including wetlands, inland waters, and rice paddies, comprising a total of 131 different ecosystems, and compared these with measurements and estimates of δ2H-H2O. We found that the estimated δ2H of annual precipitation (δ2Hp) explained approximately 35 % of the observed variation in δ2H-CH4, and that the relationship between δ2H-CH4 and δ2Hp led to significant differences in the distribution of freshwater δ2H-CH4 between the northern high latitudes (60–90º N) relative to other global regions. Residual variability in δ2H-CH4 is partially explained by differences in the dominant methanogenic pathway and CH4 oxidation, as inferred from carbon isotope fractionation between CH4 and carbon dioxide (αC). Our results imply that hydrogenotrophic methanogenesis is characterized by a steeper slope of δ2H-CH4 vs. δ2Hp than acetoclastic methanogenesis, a pattern that is consistent with previous predictions. Biogeochemical sources of variability in δ2H-CH4 are reflected in apparent differences between different freshwater ecosystems, with relatively high values in rivers and bogs, and low values in fens and rice paddies, although more data is needed to verify whether these differences are significant. To estimate how changes in the spatial distribution of freshwater emissions would influence global atmospheric CH4 isotopic measurements, we developed a bottom-up mixing model of global CH4 δ2H and δ13C sources, including spatially resolved signatures for freshwater CH4 sources. This model implies that changes in high-latitude freshwater CH4 emissions would have an especially strong influence on global source δ2H-CH4. We estimate that global CH4 emissions sources have a combined δ2H value of −277±8 ‰, which is consistent with top-down estimates based on atmospheric measurements. In contrast our estimated δ13C value of −56.4±1.4 ‰ is not consistent with atmospheric measurements, suggesting possible errors in either emissions inventories or estimates of sink fluxes and isotopic fractionations. Overall our results emphasize the value of δ2H-CH4 measurements to help constrain atmospheric CH4 budgets.

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Variability and quasi-decadal changes in the methane budget over the period 2000–2012

10.5194/acp-2017-296 ◽

2017 ◽

Cited By ~ 2

Author(s):

Marielle Saunois ◽

Philippe Bousquet ◽

Benjamin Poulter ◽

Anna Peregon ◽

Philippe Ciais ◽

...

Keyword(s):

Biomass Burning ◽

Methane Emissions ◽

Data Driven ◽

Atmospheric Methane ◽

Top Down ◽

Bottom Up ◽

Ch4 Emissions ◽

Ensemble Mean ◽

The Mean ◽

The Tropics

Abstract. Following the recent Global Carbon project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling frameworks) and bottom-up models, inventories, and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seems to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the EDGARv4.2 inventory, which should be revised to smaller values in a near future. Though the sectorial partitioning of six individual top-down studies out of eight are not consistent with the observed change in atmospheric 13CH4, the partitioning derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that, the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. Besides, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. The methane loss (in particular through OH oxidation) has not been investigated in detail in this study, although it may play a significant role in the recent atmospheric methane changes.

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Exploring Gaps between Bottom-Up and Top-Down Emission Estimates Based on Uncertainties in Multiple Emission Inventories: A Case Study on CH4 Emissions in China

Sustainability ◽

10.3390/su11072054 ◽

2019 ◽

Vol 11 (7) ◽

pp. 2054 ◽

Cited By ~ 6

Author(s):

Penwadee Cheewaphongphan ◽

Satoru Chatani ◽

Nobuko Saigusa

Keyword(s):

Coal Mining ◽

Rice Cultivation ◽

Emission Inventories ◽

Ch4 Emission ◽

Top Down ◽

Activity Data ◽

Bottom Up ◽

Ch4 Emissions ◽

Model Studies ◽

Livestock Sector

Bottom-up CH4 emission inventories, which have been developed from statistical analyses of activity data and country specific emission factors (EFs), have high uncertainty in terms of the estimations, according to results from top-down inverse model studies. This study aimed to determine the causes of overestimation in CH4 bottom-up emission inventories across China by applying parameter variability uncertainty analysis to three sets of CH4 emission inventories titled PENG, GAINS, and EDGAR. The top three major sources of CH4 emissions in China during the years 1990–2010, namely, coal mining, livestock, and rice cultivation, were selected for the investigation. The results of this study confirm the concerns raised by inverse modeling results in which we found significantly higher bottom-up emissions for the rice cultivation and coal mining sectors. The largest uncertainties were detected in the rice cultivation estimates and were caused by variations in the proportions of rice cultivation ecosystems and EFs; specifically, higher rates for both parameters were used in EDGAR. The coal mining sector was associated with the second highest level of uncertainty, and this was caused by variations in mining types and EFs, for which rather consistent parameters were used in EDGAR and GAINS, but values were slightly higher than those used in PENG. Insignificant differences were detected among the three sets of inventories for the livestock sector.

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Inverse modelling of European CH<sub>4</sub> emissions during 2006–2012 using different inverse models and reassessed atmospheric observations

10.5194/acp-2017-273 ◽

2017 ◽

Cited By ~ 2

Author(s):

Peter Bergamaschi ◽

Ute Karstens ◽

Alistair J. Manning ◽

Marielle Saunois ◽

Aki Tsuruta ◽

...

Keyword(s):

A Priori ◽

Lower Troposphere ◽

Inverse Modelling ◽

Top Down ◽

Data Set ◽

Bottom Up ◽

Ch4 Emissions ◽

In Situ Data ◽

Inverse Models ◽

The Impact

Abstract. We present inverse modelling (top-down) estimates of European methane (CH4) emissions for 2006–2012 based on a new quality-controlled and harmonized in-situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.7 (20.2–29.7) Tg CH4 yr−1 (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006–2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom-up, based on statistical data and emissions factors) amount to only 21.3 Tg CH4 yr−1 (2006) to 18.8 Tg CH4 yr−1 (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP) total wetland emissions of 4.3 (2.3–8.2) CH4 yr−1 from EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. This analysis identifies regional biases for several models at the aircraft profile sites in France, Hungary and Poland.

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The Global Methane Budget 2000–2017

Earth System Science Data ◽

10.5194/essd-12-1561-2020 ◽

2020 ◽

Vol 12 (3) ◽

pp. 1561-1623 ◽

Cited By ~ 33

Author(s):

Marielle Saunois ◽

Ann R. Stavert ◽

Ben Poulter ◽

Philippe Bousquet ◽

Josep G. Canadell ◽

...

Keyword(s):

Climate Change ◽

Land Surface ◽

Anthropogenic Emissions ◽

Inland Waters ◽

Top Down ◽

Bottom Up ◽

Methane Budget ◽

Carbon Project ◽

Global Carbon ◽

Process Based Models

Abstract. Understanding and quantifying the global methane (CH4) budget is 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 in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions 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) is 29 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 previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-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 methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological 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 overall discrepancy between bottom-up and top-down estimates has been reduced by only 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 methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from the Global Carbon Project.

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Limitations of the radon tracer method (RTM) to estimate regional greenhouse gas (GHG) emissions – a case study for methane in Heidelberg

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-17907-2021 ◽

2021 ◽

Vol 21 (23) ◽

pp. 17907-17926

Author(s):

Ingeborg Levin ◽

Ute Karstens ◽

Samuel Hammer ◽

Julian DellaColetta ◽

Fabian Maier ◽

...

Keyword(s):

Greenhouse Gas ◽

Inversion Layer ◽

Ghg Emissions ◽

Point Sources ◽

Atmospheric Methane ◽

Tracer Method ◽

Top Down ◽

Bottom Up ◽

Ch4 Emissions ◽

Annual Variations

Abstract. Correlations of nighttime atmospheric methane (CH4) and 222radon (222Rn) observations in Heidelberg, Germany, were evaluated with the radon tracer method (RTM) to estimate the trend of annual nocturnal CH4 emissions from 1996–2020 in the footprint of the station. After an initial 30 % decrease in emissions from 1996 to 2004, there was no further systematic trend but small inter-annual variations were observed thereafter. This is in accordance with the trend of total emissions until 2010 reported by the EDGARv6.0 inventory for the surroundings of Heidelberg and provides a fully independent top-down verification of the bottom-up inventory changes. We show that the reliability of total nocturnal CH4 emission estimates with the RTM critically depends on the accuracy and representativeness of the 222Rn exhalation rates estimated from soils in the footprint of the site. Simply using 222Rn fluxes as estimated by Karstens et al. (2015) could lead to biases in the estimated greenhouse gas (GHG) fluxes as large as a factor of 2. RTM-based GHG flux estimates also depend on the parameters chosen for the nighttime correlations of CH4 and 222Rn, such as the nighttime period for regressions and the R2 cut-off value for the goodness of the fit. Quantitative comparison of total RTM-based top-down flux estimates with bottom-up emission inventories requires representative high-resolution footprint modelling, particularly in polluted areas where CH4 emissions show large heterogeneity. Even then, RTM-based estimates are likely biased low if point sources play a significant role in the station footprint as their emissions may not be fully captured by the RTM method, for example, if stack emissions are injected above the top of the nocturnal inversion layer or if point-source emissions from the surface are not well mixed into the footprint of the measurement site. Long-term representative 222Rn flux observations in the footprint of a station are indispensable in order to apply the RTM method for reliable quantitative flux estimations of GHG emissions from atmospheric observations.

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The carbon budget of South Asia

Biogeosciences ◽

10.5194/bg-10-513-2013 ◽

2013 ◽

Vol 10 (1) ◽

pp. 513-527 ◽

Cited By ~ 58

Author(s):

P. K. Patra ◽

J. G. Canadell ◽

R. A. Houghton ◽

S. L. Piao ◽

N.-H. Oh ◽

...

Keyword(s):

South Asia ◽

South Asian ◽

Co2 Flux ◽

Terrestrial Ecosystems ◽

Top Down ◽

Bottom Up ◽

Ch4 Emissions ◽

Asian Region ◽

Co2 Equivalent ◽

South Asian Region

Abstract. The source and sinks of carbon dioxide (CO2) and methane (CH4) due to anthropogenic and natural biospheric activities were estimated for the South Asian region (Bangladesh, Bhutan, India, Nepal, Pakistan and Sri Lanka). Flux estimates were based on top-down methods that use inversions of atmospheric data, and bottom-up methods that use field observations, satellite data, and terrestrial ecosystem models. Based on atmospheric CO2 inversions, the net biospheric CO2 flux in South Asia (equivalent to the Net Biome Productivity, NBP) was a sink, estimated at −104 ± 150 Tg C yr−1 during 2007–2008. Based on the bottom-up approach, the net biospheric CO2 flux is estimated to be −191 ± 193 Tg C yr−1 during the period of 2000–2009. This last net flux results from the following flux components: (1) the Net Ecosystem Productivity, NEP (net primary production minus heterotrophic respiration) of −220 ± 186 Tg C yr−1 (2) the annual net carbon flux from land-use change of −14 ± 50 Tg C yr−1, which resulted from a sink of −16 Tg C yr−1 due to the establishment of tree plantations and wood harvest, and a source of 2 Tg C yr−1 due to the expansion of croplands; (3) the riverine export flux from terrestrial ecosystems to the coastal oceans of +42.9 Tg C yr−1; and (4) the net CO2 emission due to biomass burning of +44.1 ± 13.7 Tg C yr−1. Including the emissions from the combustion of fossil fuels of 444 Tg C yr−1 for the 2000s, we estimate a net CO2 land–atmosphere flux of 297 Tg C yr−1. In addition to CO2, a fraction of the sequestered carbon in terrestrial ecosystems is released to the atmosphere as CH4. Based on bottom-up and top-down estimates, and chemistry-transport modeling, we estimate that 37 ± 3.7 Tg C yr−1 were released to atmosphere from South Asia during the 2000s. Taking all CO2 and CH4 fluxes together, our best estimate of the net land–atmosphere CO2-equivalent flux is a net source of 334 Tg C yr−1 for the South Asian region during the 2000s. If CH4 emissions are weighted by radiative forcing of molecular CH4, the total CO2-equivalent flux increases to 1148 Tg C yr−1 suggesting there is great potential of reducing CH4 emissions for stabilizing greenhouse gases concentrations.

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Inverse modelling of European CH<sub>4</sub> emissions during 2006–2012 using different inverse models and reassessed atmospheric observations

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-901-2018 ◽

2018 ◽

Vol 18 (2) ◽

pp. 901-920 ◽

Cited By ~ 23

Author(s):

Peter Bergamaschi ◽

Ute Karstens ◽

Alistair J. Manning ◽

Marielle Saunois ◽

Aki Tsuruta ◽

...

Keyword(s):

Regional Distribution ◽

Inverse Modelling ◽

Top Down ◽

Data Set ◽

Bottom Up ◽

Natural Sources ◽

Ch4 Emissions ◽

Inverse Models ◽

The Impact ◽

The Eu

Abstract. We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006–2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.8 (20.2–29.7) Tg CH4 yr−1 (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006–2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 Tg CH4 yr−1 (2006) to 18.8 Tg CH4 yr−1 (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3–8.2) Tg CH4 yr−1 from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. The estimated average regional biases range between −40 and 20 % at the aircraft profile sites in France, Hungary and Poland.

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The carbon budget of South Asia

Biogeosciences Discussions ◽

10.5194/bgd-9-13537-2012 ◽

2012 ◽

Vol 9 (10) ◽

pp. 13537-13580

Author(s):

P. K. Patra ◽

J. G. Canadell ◽

R. A. Houghton ◽

S. L. Piao ◽

N.-H. Oh ◽

...

Keyword(s):

South Asia ◽

Radiative Forcing ◽

Net Primary Production ◽

Co2 Flux ◽

Terrestrial Ecosystems ◽

The South ◽

Top Down ◽

Bottom Up ◽

Ch4 Emissions ◽

Co2 Equivalent

Abstract. The source and sinks of carbon dioxide (CO2) and methane (CH4) due to anthropogenic and natural biospheric activities were estimated for the South Asia region (Bangladesh, Bhutan, India, Nepal, Pakistan and Sri Lanka). Flux estimates were based on top-down methods that use inversions of atmospheric data, and bottom-up methods that use field observations, satellite data, and terrestrial ecosystem models. Based on atmospheric CO2 inversions, the net biospheric CO2 flux in South Asia (equivalent to the Net Biome Productivity, NBP) was a sink, estimated at −104 ± 150 Tg C yr−1 during 2007–2008. Based on the bottom-up approach, the net biospheric CO2 flux is estimated to be −191 ± 193 Tg C yr−1 during the period of 2000–2009. This last net flux results from the following flux components: (1) the Net Ecosystem Productivity, NEP (net primary production minus heterotrophic respiration) of −220 ± 186 Tg C yr−1 (2) the annual net carbon flux from land-use change of −14 ± 50 Tg C yr−1, which resulted from a sink of −16 Tg C yr−1 due to the establishment of tree plantations and wood harvest, and a source of 2 Tg C yr−1 due to the expansion of croplands; (3) the riverine export flux from terrestrial ecosystems to the coastal oceans of +42.9 Tg C yr−1; and (4) the net CO2 emission due to biomass burning of +44.1 ± 13.7 Tg C yr−1. Including the emissions from the combustion of fossil fuels of 444 Tg C yr−1 for the decades of 2000s, we estimate a net CO2 land-to-atmosphere flux of 297 Tg C yr−1. In addition to CO2, a fraction of the sequestered carbon in terrestrial ecosystems is released to the atmosphere as CH4. Based on bottom-up and top-down estimates, and chemistry-transport modeling, we estimate that 37 ± 3.7 Tg C-CH4 yr−1 were released to atmosphere from South Asia during the 2000s. Taking all CO2 and CH4 fluxes together, our best estimate of the net land-to-atmosphere CO2-equivalent flux is a net source of 334 Tg C yr−1 for the South Asia region during the 2000s. If CH4 emissions are weighted by radiative forcing of molecular CH4, the total CO2-equivalent flux increases to 1148 Tg C yr−1 suggesting there is great potential of reducing CH4 emissions for stabilizing greenhouse gases concentrations.

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Conflicting estimates of natural geologic methane emissions

Elem Sci Anth ◽

10.1525/elementa.2021.00031 ◽

2021 ◽

Vol 9 (1) ◽

Author(s):

B. F. Thornton ◽

G. Etiope ◽

S. Schwietzke ◽

A. V. Milkov ◽

R. W. Klusman ◽

...

Keyword(s):

Fossil Fuel ◽

Ice Cores ◽

Methane Emissions ◽

Ch4 Emission ◽

Top Down ◽

Bottom Up ◽

Ch4 Emissions ◽

Emission Estimate

Global bottom-up and top-down estimates of natural, geologic methane (CH4) emissions (average approximately 45 Tg yr–1) have recently been questioned by near-zero (approximately 1.6 Tg yr–1) estimates based on measurements of 14CH4 trapped in ice cores, which imply that current fossil fuel industries’ CH4 emissions are underestimated by 25%–40%. As we show here, such a global near-zero geologic CH4 emission estimate is incompatible with multiple independent, bottom-up emission estimates from individual natural geologic seepage areas, each of which is of the order of 0.1–3 Tg yr–1. Further research is urgently needed to resolve the conundrum before rejecting either method or associated emission estimates in global CH4 accounting.

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