The influence of methane oxidation on the stable isotopic composition of methane emitted from Florida swamp forests

https://doi.org/10.1016/0016-7037(94)90341-7Get rights and content

Abstract

This study reports the first measurements of the δ13C of CH4 emitted from seasonally flooded swamp forests in the southeastern United States. The seasonally averaged δ13C of CH4 emitted from a north Florida swamp forest located in the St. Marks National Wildlife Refuge was −52.7 ± 6.11%. (error is ± one standard deviation throughout, n = 28), a value 13C-enriched, relative to typical wetland emissions. In an Everglades cypress dome, the average δ13C of emitted CH4 was −52.5 ± 6.7%.(n = 3). Consistent with attenuation of CH4 emission by CH4 oxidation in these environments, CH4 emitted via diffusion from the St. Marks swamp forest was enriched in 13C by 6.4 ± 5.8%. (n = 28) and D by 57 ± 36%. (n = 6) relative to sedimentary CH4. Methane emitted from the cypress dome had also been altered by oxidation, as it was enriched in 13C by 12.1 ± 4.3%. relative to sedimentary CH4. Emission experiments, performed in situ with inhibitors of aerobic CH4 oxidizing bacteria, were used to calculate the fractionation factors (α) for stable carbon and hydrogen isotopes of CH4 undergoing transport and oxidation. Values ranged from 1.003 to 1.021 and 1.050 to 1.129, respectively. The best estimates for carbon and hydrogen α values were 1.020 and 1.068, respectively. The δ values of produced (sedimentary) CH4 were relatively constant in the St. Marks subtropical swamp forest. Additionally, because the transport of CH4 to the atmosphere was dominated by molecular diffusion, variations in the magnitude of CH4 oxidation appeared to be the primary factor controlling the δ values of emitted CH4. This contrasts with systems dominated by bubble ebullition, where variations in CH4 production mechanisms have been hypothesized to be the primary factor controlling the δ values of emitted CH4.

References (57)

  • C Bedard et al.

    Physiology, biochemistry, and specific inhibitors of CH4, NH+4 and CO oxidation by methanotrophs and nitrifiers

    Microbiol. Rev.

    (1989)
  • N.E Blair et al.

    Carbon isotope fractionation in heterotrophic microbial metabolism

    Appl. Environ. Microbiol

    (1985)
  • N.E Blair et al.

    Natural abundances of carbon isotopes in acetate from a coastal marine sediment

    Science

    (1987)
  • N.E Blair et al.

    The carbon isotope biogeochemistry of methane production in anoxic sediments. 1. Field observations

  • R.A Burke et al.

    Seasonal variations of D/H and 13C12C ratios of microbial methane in surface sediments

    Nature

    (1988)
  • R.A Burke et al.

    Seasonal variations of stable hydrogen and carbon isotope ratios of methane in subtropical freshwater sediments

    Global Biogeochem. Cycles

    (1992)
  • J.P Chanton et al.

    Seasonal variations in ebullitive flux and carbon isotopic composition of methane in a tidal freshwater estuary

    Global Biogeochem. Cycles

    (1988)
  • J.P Chanton et al.

    Seasonal variations in the isotopic composition of methane associated with aquatic emergent macrophytes of the central Amazon basin

  • J.P Chanton et al.

    Carbon isotopic composition of methane in Florida Everglades soils and fractionation during its transport to the troposhpere

    Global Biogeochem. Cycles

    (1988)
  • J.P Chanton et al.

    Amazon Capims (floating grassmats): A source of 13C enriched methane to the troposphere

    Geophys. Res. Lett.

    (1989)
  • J.P Chanton et al.

    Gas transport from methane-saturated, tidal freshwater and wetland sediments

    Limnol. Oceanogr.

    (1989)
  • J.P Chanton et al.

    Mechanism of methane transport and isotope fractionation in macrophytes of Alaskan tundra lakes

    J. Geophys. Res.

    (1992)
  • J.P Chanton et al.

    Methane flux from Peltandra virginica: Stable isotope tracing and chamber effects

    Global Biogeochem. Cycles

    (1992)
  • J.P Chanton et al.

    Aquatic macrophyte gas transport mechanisms revealed by methane stable isotopic analysis

    Abstracts: Amer. Soc. Limnol. Oceanogr

    (1992)
  • R.J Cicerone et al.

    Methane emissions from California rice paddies with varied treatments

    Global Biogeochem. Cycles

    (1992)
  • A.H Devol et al.

    Methane emissions to the troposphere from the Amazon floodplain

    J. Geophys. Res.

    (1988)
  • A.H Devol et al.

    Seasonal dynamics in methane emissions from the Amazon River floodplain to the troposphere

    J. Geophys. Res.

    (1990)
  • I Friedman et al.

    Isotopic composition of atmospheric hydrogen

    J. Geophys. Res.

    (1974)
  • Cited by (100)

    • Extreme methane clumped isotopologue bio-signatures of aerobic and anaerobic methanotrophy: Insights from the Lake Pavin and the Black Sea sediments

      2022, Geochimica et Cosmochimica Acta
      Citation Excerpt :

      Note that when extrapolated from natural environments, kinetic isotope fractionation factors often tend to be closer to 1, representing less of a kinetic fractionation. For example, 13α values of 0.996 and Dα values of 0.952 have been reported (e.g. Happell et al., 1994). In the Lake Pavin, the methane oxidation occurs at a water depth ranging between 50 and 60 m (Lopes et al., 2011).

    • A novel belowground in-situ gas labeling approach: CH<inf>4</inf> oxidation in deep peat using passive diffusion chambers and <sup>13</sup>C excess

      2022, Science of the Total Environment
      Citation Excerpt :

      The first group of methods is based on carbon (C) and hydrogen (H) stable isotope composition. Here, CH4 oxidation shifts the stable isotope composition because methanotrophs discriminate strongly against heavier 13C and 2H isotopes during metabolism (Bellisario et al., 1999; Happell et al., 1994). This leads to accumulation of CH4 with higher δ13C and δD values as compared with those typical for methanogenesis (Whiticar, 1999).

    • Multiple stable isotopic signatures corroborate the predominance of acetoclastic methanogenesis during CH<inf>4</inf> formation in agricultural river networks

      2020, Agriculture, Ecosystems and Environment
      Citation Excerpt :

      The stable carbon (C) isotopic composition of CH4 has been used extensively in the identification of its production pathways (Conrad, 2005; Whiticar, 1999; Whiticar et al., 1986), including AM and HM (Chanton et al., 2005; Whiticar et al., 1986). Furthermore, stable hydrogen (H) (D, deuterium, i.e., 2H) isotopes can be combined with stable C isotopes and used to diagnose sources of CH4 (Whiticar et al., 1986), and also be used to quantify the influence of microbial oxidation in freshwater environments (Coleman et al., 1981; Happell et al., 1994). Hence, isotopic information is especially useful as a direct means of constraining and interpreting temporal variations in the CH4 budget due to the characteristic isotope ratios associated with the major CH4 sources: wetlands, rice paddies, and ruminants, δ13C ∼ –60‰ and δD ∼ –300‰; fugitive fossil fuels, δ13C ∼ –40‰and δD ∼ –175‰; and biomass-burning, δ13C ∼ –20‰ and δD ∼ –200‰ (Rice et al., 2016).

    View all citing articles on Scopus
    View full text