Centennial evolution of the atmospheric methane budget: what do the carbon isotopes tell us?
Open Access
- 2 May 2007
- journal article
- Published by Copernicus GmbH in Atmospheric Chemistry and Physics
- Vol. 7 (8) , 2119-2139
- https://doi.org/10.5194/acp-7-2119-2007
Abstract
Little is known about how the methane source inventory and sinks have evolved over recent centuries. New and detailed records of methane mixing ratio and isotopic composition (12CH4, 13CH4 and 14CH4) from analyses of air trapped in polar ice and firn can enhance this knowledge. We use existing bottom-up constructions of the source history, including "EDGAR"-based constructions, as inputs to a model of the evolving global budget for methane and for its carbon isotope composition through the 20th century. By matching such budgets to atmospheric data, we examine the constraints imposed by isotope information on those budget evolutions. Reconciling both 12CH4 and 13CH4 budgets with EDGAR-based source histories requires a combination of: a greater proportion of emissions from biomass burning and/or of fossil methane than EDGAR constructions suggest; a greater contribution from natural such emissions than is commonly supposed; and/or a significant role for active chlorine or other highly-fractionating tropospheric sink as has been independently proposed. Examining a companion budget evolution for 14CH4 exposes uncertainties in inferring the fossil-methane source from atmospheric 14CH4 data. Specifically, methane evolution during the nuclear era is sensitive to the cycling dynamics of "bomb 14C" (originating from atmospheric weapons tests) through the biosphere. In addition, since ca. 1970, direct production and release of 14CH4 from nuclear-power facilities is influential but poorly quantified. Atmospheric 14CH4 determinations in the nuclear era have the potential to better characterize both biospheric carbon cycling, from photosynthesis to methane synthesis, and the nuclear-power source.Keywords
All Related Versions
This publication has 103 references indexed in Scilit:
- Methane emissions from terrestrial plants under aerobic conditionsNature, 2006
- CH4 sources estimated from atmospheric observations of CH4 and its 13C/12C isotopic ratios: 2. Inverse modeling of CH4 fluxes from geographical regionsGlobal Biogeochemical Cycles, 2004
- Interannual variability and trend of CH4 lifetime as a measure for OH changes in the 1979–1993 time periodJournal of Geophysical Research: Atmospheres, 2003
- AGE OF STRATOSPHERIC AIR: THEORY, OBSERVATIONS, AND MODELSReviews of Geophysics, 2002
- Reconstructing atmospheric histories from measurements of air composition in firnJournal of Geophysical Research: Atmospheres, 2002
- Development of analytical methods and measurements of 13C/12C in atmospheric CH4 from the NOAA Climate Monitoring and Diagnostics Laboratory Global Air Sampling NetworkJournal of Geophysical Research: Atmospheres, 2002
- Shipboard determinations of the distribution of 13C in atmospheric methane in the PacificJournal of Geophysical Research: Atmospheres, 1999
- Inverse modeling of methane sources and sinks using the adjoint of a global transport modelJournal of Geophysical Research: Atmospheres, 1999
- Controls on CH4 emissions from a northern peatlandGlobal Biogeochemical Cycles, 1999
- Carbon kinetic isotope effect in the reaction of CH4 with Cl atomsGeophysical Research Letters, 1995