Vertical Hydrologic Exchange Flows Control Methane Emissions from Riverbed Sediments

Abstract

CH₄ emissions from inland waters are highly uncertain in the current global CH₄ budget, especially for streams, rivers, and other lotic systems. Previous studies have attributed the strong spatiotemporal heterogeneity of riverine CH₄ to environmental factors such as sediment type, water level, temperature, or particulate organic carbon abundance through correlation analysis. However, a mechanistic understanding of the basis for such heterogeneity is lacking. Here, we combine sediment CH₄ data from the Hanford reach of the Columbia River with a biogeochemical-transport model to show that vertical hydrologic exchange flows (VHEFs), driven by the difference between river stage and groundwater level, determine CH₄ flux at the sediment-water interface. CH₄ fluxes show a nonlinear relationship with the magnitude of VHEFs, where high VHEFs introduce O₂ into riverbed sediments, which inhibit CH₄ production and induce CH₄ oxidation, and low VHEFs cause transient reduction in CH₄ flux (relative to production) due to reduced advective CH₄ transport. In addition, VHEFs lead to the hysteresis of temperature rise and CH₄ emissions because high river discharge caused by snowmelt in spring leads to strong downwelling flow that offsets increasing CH₄ production with temperature rise. Our findings reveal how the interplay between in-stream hydrologic flux besides fluvial-wetland connectivity and microbial metabolic pathways that compete with methanogenic pathways can produce complex patterns in CH₄ production and emission in riverbed alluvial sediments.

Keywords: microbial-explicit model; riverine CH4 emission; sediment biogeochemical cycling; temperature hysteresis; vertical hydrologic exchange flows.