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2. Evolution of the Oceanic ¹³ C Suess Effect in the Southeastern Indian Ocean Between 1994 and 2018

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4. Impacts of Carbonate Buffering on Atmospheric Equilibration of CO ₂ , δ ¹³ C _DIC , and Δ ¹⁴ C _DIC in Rivers and Streams

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   Winnick, Matthew J.; Saccardi, Brian (February 2024, Global Biogeochemical Cycles)

   Abstract Rivers and streams play an important role within the global carbon cycle, in part through emissions of carbon dioxide (CO₂) to the atmosphere. However, the sources of this CO₂and their spatiotemporal variability are difficult to constrain. Recent work has highlighted the role of carbonate buffering reactions that may serve as a source of CO₂in high alkalinity systems. In this study, we seek to develop a quantitative framework for the role of carbonate buffering in the fluxes and spatiotemporal patterns of CO₂and the stable and radio‐ isotope composition of dissolved inorganic carbon (DIC). We incorporate DIC speciation calculations of carbon isotopologues into a stream network CO₂model and perform a series of simulations, ranging from the degassing of a groundwater seep to a hydrologically‐coupled 5th‐order stream network. We find that carbonate buffering reactions contribute >60% of emissions in high‐alkalinity, moderate groundwater‐CO₂environments. However, atmosphere equilibration timescales of CO₂are minimally affected, which contradicts hypotheses that carbonate buffering maintains high CO₂across Strahler orders in high alkalinity systems. In contrast, alkalinity dramatically increases isotope equilibration timescales, which acts to decouple CO₂and DIC variations from the isotopic composition even under low alkalinity. This significantly complicates a common method for carbon source identification. Based on similar impacts on atmospheric equilibration for stable and radio‐ carbon isotopologues, we develop a quantitative method for partitioning groundwater and stream corridor carbon sources in carbonate‐dominated watersheds. Together, these results provide a framework to guide fieldwork and interpretations of stream network CO₂patterns across variable alkalinities. 

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