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Sulfur isotopes in rivers : insights into global weathering budgets, pyrite oxidation, and the modern sulfur cycle (2018)

Burke, Andrea ; Present, Theodore M. ; Paris, Guillaume ; [et al.]

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Publication Date: 2022-05-25

Description: Author Posting. © The Author(s), 2018. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Earth and Planetary Science Letters 496 (2018): 168-177, doi:10.1016/j.epsl.2018.05.022.

Description: The biogeochemical sulfur cycle is intimately linked to the cycles of carbon, iron, and oxygen, and plays an important role in global climate via weathering reactions and aerosols. However, many aspects of the modern budget of the global sulfur cycle are not fully understood. We present new δ34S measurements on sulfate from more than 160 river samples from different geographical and climatic regions—more than 46% of the world’s freshwater flux to the ocean is accounted for in this estimate of the global riverine sulfur isotope budget. These measurements include major rivers and their tributaries, as well as time series, and are combined with previously published data to estimate the modern flux-weighted global riverine δ34S as 4.4 ± 4.5 ‰ (V-CDT), and 4.8 ± 4.9 ‰ when the most polluted rivers are excluded. Combined with major anion and cation concentrations, the sulfur isotope data allow us to tease apart the relative contributions of different processes to the modern riverine sulfur budget, resulting in new estimates of the flux of riverine sulfate due to the oxidative weathering of pyrites (1.3 ± 0.2 Tmol S/y) and the weathering of sedimentary sulfate minerals (1.5 ± 0.2 Tmol S/y). These data indicate that previous estimates of the global oxidative weathering of pyrite have been too low by a factor of two. As pyrite oxidation coupled to carbonate weathering can act as a source of CO2 to the atmosphere, this global pyrite weathering budget implies that the global CO2 weathering sink is overestimated. Furthermore, the large range of sulfur isotope ratios in modern rivers indicates that secular changes in the lithologies exposed to weathering through time could play a major role in driving past variations in δ34S of seawater.

Description: This research was funded by a Foster and Coco Stanback postdoctoral fellowship and a Marie Curie Career Integration Grant (CIG14-631752) to AB. JFA acknowledges the support of NSF-OCE grant 1340174 and NSF-EAR grant 1349858. WF acknowledges the support of a grant from the David and Lucile Packard Foundation.

Keywords: Sulfur ; Rivers ; Weathering ; Pyrite

Repository Name: Woods Hole Open Access Server

Type: Preprint

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Particulate organic carbon and nitrogen export from major Arctic rivers (2016)

McClelland, James W. ; Holmes, Robert M. ; Peterson, Bruce J. ; [et al.]

John Wiley & Sons

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Publication Date: 2022-05-26

Description: Author Posting. © American Geophysical Union, 2016. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 30 (2016): 629–643, doi:10.1002/2015GB005351.

Description: Northern rivers connect a land area of approximately 20.5 million km2 to the Arctic Ocean and surrounding seas. These rivers account for ~10% of global river discharge and transport massive quantities of dissolved and particulate materials that reflect watershed sources and impact biogeochemical cycling in the ocean. In this paper, multiyear data sets from a coordinated sampling program are used to characterize particulate organic carbon (POC) and particulate nitrogen (PN) export from the six largest rivers within the pan-Arctic watershed (Yenisey, Lena, Ob', Mackenzie, Yukon, Kolyma). Together, these rivers export an average of 3055 × 109 g of POC and 368 × 109 g of PN each year. Scaled up to the pan-Arctic watershed as a whole, fluvial export estimates increase to 5767 × 109 g and 695 × 109 g of POC and PN per year, respectively. POC export is substantially lower than dissolved organic carbon export by these rivers, whereas PN export is roughly equal to dissolved nitrogen export. Seasonal patterns in concentrations and source/composition indicators (C:N, δ13C, Δ14C, δ15N) are broadly similar among rivers, but distinct regional differences are also evident. For example, average radiocarbon ages of POC range from ~2000 (Ob') to ~5500 (Mackenzie) years before present. Rapid changes within the Arctic system as a consequence of global warming make it challenging to establish a contemporary baseline of fluvial export, but the results presented in this paper capture variability and quantify average conditions for nearly a decade at the beginning of the 21st century.

Description: National Science Foundation Grant Numbers: 0229302, 0732985; U.S. Geological Survey; Department of Indian and Northern Affairs

Description: 2016-11-11

Keywords: Arctic ; River ; Carbon ; Nitrogen ; Watershed ; Export