Coupling of stable carbon isotopic signature of methane and ebullitive fluxes in northern temperate lakes

Publications

Coupling of stable carbon isotopic signature of methane and ebullitive fluxes in northern temperate lakes

Year : 2021

Publisher : Elsevier B.V.

Source Title : Science of the Total Environment

Document Type :

Abstract

Stable isotopic analysis is a popular method to understand the mechanisms sustaining methane (CH4) emissions in various aquatic environments. Yet, the general lack of concurrent measurements of isotopes and fluxes impedes our ability to establish a connection between the variation in the rates of CH4 emission and isotopic signature. Here, we examine the magnitude of CH4 ebullition (bubbling) and stable carbon isotopic signature (δ13C-CH4) of bubble CH4 in four northern temperate lakes and evaluate the in-lake processes shaping their variability. The ebullitive CH4 flux and bubble δ13C-CH4 varied from 0.01 to 37.0 mmol m−2 d−1 and between −71.0‰ and −50.9‰, respectively. The high emission lakes in general and high fluxing shallow zones within each lake consistently showed enriched δ13C-CH4 signature. Subsequently, in addition to the temperature dependence (1.4 ± 0.1 eV), the rates of ebullition strongly correlated with the variability of δ13C-CH4 across our study lakes. Our results suggest that higher ebullitive emissions are sustained by acetoclastic methanogenesis, likely fueled by fresh organic matter inputs. Further, the annual whole-lake estimate of bubble isotopic flux alone showed depleted δ13C-CH4 values (−64.6 ± 0.6‰ to −60.1 ± 3.2‰), yet the signature of the total CH4 emission (ebullition + diffusion) was relatively enriched (−60.7‰ to −52.6‰) due to high methanotrophic activity in the water column. We show that δ13C-CH4 signature of bubbles can be linked to the magnitude of ebullition itself, yet we suggest there is a need to account for different emission pathways and their isotopic signature to allocate CH4 source signature to northern lakes.