Carbon isotopic composition of atmospheric CH4: Fossil and biomass burning source strengths

Abstract

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 and 1989. The global average δ13CPDB from these measurements (n = 208) was −47.20 ± 0.13%o. The lowest mean annual δ13C value of‐47.61 ± 0.14‰ was measured at Point Barrow with values increasing to ‐47.03 ± 0.14‰ at Cape Grim. The seasonal cycle in the δ13C of CH4 was greatest at Point Barrow, with an amplitude of 0.5‰, 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 δ13C 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−1, 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 δ13C of −47.2‰, when coupled with the 14C results, implies that ∼11% of the total CH4 release rate is derived from biomass burning. These results indicate for a total CH4 source of ∼550 Tg yr−1 that natural gas release accounts for ∼90 Tg yr−1 and biomass burning yields ∼60 Tg yr−1. Preliminary analyses of the δ13C data using a three‐dimensional chemical tracer model indicate that the observed meridional gradients in the annual average δ13C and concentration of CH4 are most closely matched with a CH4 source scenario in which 11% of the CH4 is derived from biomass burning.