The biogeochemistry of methane isotopologues in marine and lacustrine sediments

Abstract

Methane is a globally significant greenhouse gas, energy resource, and it is a product and reactant of microbial metabolisms. Multiple sources and sinks of methane can be challenging to distinguish from each other, thus complicating the understanding of methane budgets and the effects of microbes on mediating Earth’s carbon cycle. The relative abundances of methane isotopologues (e.g., 12CH4, 13CH4, 12CH3D, and 13CH3D) record process-based information about the formation conditions, transport, and fate of methane, and in select environments can serve as a temperature proxy. This geochemical tool is herein applied to methane from marine and lacustrine sediments to test assumptions about prevailing mechanisms of its formation and consumption in these settings. This thesis describes 1) three studies about biogeochemical insights gained by quantifying the relative abundance of clumped methane isotopologue, 13CH3D, in samples from marine and lacustrine sediments, and 2) one foray into method development to improve the quantification of methane in these environments. Chapter 2 presents a global survey of marine gas hydrates where isotope-based temperatures are used to assess whether linkages between methane sources and seepage-associated seafloor features match putative geologic models. Chapter 3 describes two kilometer-scale profiles of methane isotopologues from marine sediments, where the relationship between expected sediment temperature and isotope-based temperature is used to evaluate the temperature limit of microbial processing and abiotic re-equilibration mechanisms. Chapter 4 reports the largest set of methane isotopologue data from ebullition in a single lake basin, which is used to gauge the relative importance of aerobic and anaerobic methane oxidation in the study site and recommend a general sampling strategy to constrain methane source signatures in similar lake settings. Chapter 5 explains the development of a method to quantify the in situ concentration of methane based on ratios of dissolved gases, and its comparison to four other methane quantification methods for surface sediments from marine cold seeps. The findings from this research contribute to ongoing efforts to understand the sedimentary carbon cycle and microbial activity in remote environments.

Methane Clumped Isotopologue Variability from Ebullition in a Mid-latitude Lake

“…This work is part of the doctoral dissertation by E.L. titled "The biogeochemistry of methane isotopologues in marine and lacustrine sediments". 82…”