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2016
Saunois, M, Bousquet P, Poulter B, Peregon A, Ciais P, Canadell JG, Dlugokencky EJ, Etiope G, Bastviken D, Houweling S, Janssens-Maenhout G, Tubiello FN, Castaldi S, Jackson RB, Alexe M, Arora VK, Beerling DJ, Bergamaschi P, Blake DR, Brailsford G, Brovkin V, Bruhwiler L, Crevoisier C, Crill P, Covey K, Curry C, Frankenberg C, Gedney N, Hoglund-Isaksson L, Ishizawa M, Ito A, Joos F, Kim HS, Kleinen T, Krummel P, Lamarque JF, Langenfelds R, Locatelli R, Machida T, Maksyutov S, McDonald KC, Marshall J, Melton JR, Morino I, Naik V, O'Doherty S, Parmentier FJW, Patra PK, Peng CH, Peng SS, Peters GP, Pison I, Prigent C, Prinn R, Ramonet M, Riley WJ, Saito M, Santini M, Schroeder R, Simpson IJ, Spahni R, Steele P, Takizawa A, Thornton BF, Tian HQ, Tohjima Y, Viovy N, Voulgarakis A, van Weele M, van der Werf GR, Weiss R, Wiedinmyer C, Wilton DJ, Wiltshire A, Worthy D, Wunch D, Xu XY, Yoshida Y, Zhang B, Zhang Z, Zhu Q.  2016.  The global methane budget 2000-2012. Earth System Science Data. 8:697-751.   10.5194/essd-8-697-2016   AbstractWebsite

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (similar to biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558 TgCH(4) yr(-1), range 540-568. About 60% of global emissions are anthropogenic (range 50-65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 TgCH(4) yr(-1), range 596-884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (similar to 64% of the global budget, <30 degrees N) as compared to mid (similar to 32 %, 30-60 degrees N) and high northern latitudes (similar to 4 %, 60-90 degrees N). Top-down inversions consistently infer lower emissions in China (similar to 58 TgCH(4) yr(-1), range 51-72, -14 %) and higher emissions in Africa (86 TgCH(4) yr(-1), range 73-108, + 19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30-40% on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.

2013
Kirschke, S, Bousquet P, Ciais P, Saunois M, Canadell JG, Dlugokencky EJ, Bergamaschi P, Bergmann D, Blake DR, Bruhwiler L, Cameron-Smith P, Castaldi S, Chevallier F, Feng L, Fraser A, Heimann M, Hodson EL, Houweling S, Josse B, Fraser PJ, Krummel PB, Lamarque JF, Langenfelds RL, Le Quere C, Naik V, O'Doherty S, Palmer PI, Pison I, Plummer D, Poulter B, Prinn RG, Rigby M, Ringeval B, Santini M, Schmidt M, Shindell DT, Simpson IJ, Spahni R, Steele LP, Strode SA, Sudo K, Szopa S, van der Werf GR, Voulgarakis A, van Weele M, Weiss RF, Williams JE, Zeng G.  2013.  Three decades of global methane sources and sinks. Nature Geoscience. 6:813-823.   10.1038/ngeo1955   AbstractWebsite

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios - which differ in fossil fuel and microbial emissions - to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

1970
Takahashi, T, Weiss RF, Culberson CH, Edmond JM, Hammond DE, Wong CS, Li Y-hui, Bainbridge AE.  1970.  A carbonate chemistry profile at the 1969 GEOSECS intercalibration station in the eastern Pacific Ocean. Journal of Geophysical Research. 75:7648-7666., Washington, DC, United States (USA): American Geophysical Union, Washington, DC   10.1029/JC075i036p07648   AbstractWebsite

To compare and evaluate measurements made by the various laboratories participating in the Geochemical Ocean Section Study (Geosecs), four carbonate chemistry parameters, pH, pCO2, alkalinity, and total dissolved CO2, as well as temperature and salinity were measured for samples collected at the Geosecs intercalibration station, 28°20′±07′N and 121°41′±02′W. The methods for measurement include the glass-calomel electrode pair for pH, the pH and the potentiometric acid titration methods for alkalinity, gas chromatographic, infrared and potentiometric acid titration method for total CO2, and the gas equilibrator-infrared method for pCO2. The alkalinity values measured by the pH method agree with the values measured by the potentiometric acid titration method within 1%, and the total CO2 values measured by the chromatographic method agree with the values measured by the potentiometric acid titration method within 2%. The observed 3 to 5% difference between the total CO2 values measured by the chromatographic and infrared methods is attributed to the biological alteration of the unpoisoned samples used for the infrared methods. When two of the four measured carbonate parameters were used to calculate the remaining two parameters, the calculated values are found to differ systematically from the measured values for those two parameters. Such a discrepancy can be eliminated if a 30% error in the second apparent dissociation constant for carbonic acid (K2′) is assumed.