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ABSTRACT

Quay et al. 1991

Quay, P.D., S.L. King, J. Stutsman, D.O. Wilbur, L.P. Steele, I. Fung, R.H. Gammon, T.A. Brown, G.W. Farwell, P.M. Grootes, and F.H. Schmidt, 1991: Carbon isotopic composition of atmospheric CH4: Fossil and biomass burning source and strengths. Global Biogeochem. Cycles, 5, 25-47, doi:10.1029/91GB00003.

The 13C/12C of atmospheric methane (CH4) was measured at Point Barrow 71°N, 156°W), Olympic Peninsula (48°N, 126°W), Mauna Loa (19°N, 155°W), and Cape Grim (41°S, 144°E) between 1987 amd 1989. The global average delta-13CPDB from these measurements (n = 208) was -47.20±0.13 per mill. The lowest mean annual delta-13C value of 47.61±0.14 per mill was measured at Point Barrow with values increasing to -47.03±0.14 per mill at Cape Grim. The seasonal cycle in the delta-13C of CH4 was greatest at Point Barrow, with an amplitude of 0.5 per mill, and varied inversely with concentration. The isotopic fractionation during CH4 oxidation is calculated to be 0.993±0.002 based on the measured CH4 concentration and delta-13C values. The 14C content of atmospheric CH4, measured at monthly intervals at the Olympic Peninsula site between 1987 and 1989, is increasing at 1.4±0.5 pM/yr, primarily owing to 14CH4 release from nuclear reactors. The global average 14C content of 122 pM for CH4 implies a fossil methane source strength that is 16% of the total source. The global mean delta-13C of 47.2 per mill, when coupled with the 14C results, implies that ~11% is derived from biomass burning. These results indicate for a total CH4 source of ~550 Tg/yr that natural gas release accounts for ~90 Tg/yr and biomass burning yields ~60 Tg/yr. Preliminary analyses of the delta-13C data using a three-dimensional chemical tracer model indicate that the observed meridional gradients in the annual average delta-13C and concentration of CH4 are most closely matched with a CH4 source scenario in which 11% of the CH4 is derived from biomass burning.

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