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  • 1
    Publication Date: 2022-10-26
    Description: Author Posting. © American Geophysical Union, 2021. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research: Biogeosciences 126(7), (2021): e2020JG005977, https://doi.org/10.1029/2020JG005977.
    Description: Increasing Arctic temperatures are thawing permafrost soils and liberating ancient organic matter, but the fate of this material remains unclear. Thawing of permafrost releases dissolved organic matter (DOM) into fluvial networks. Unfortunately, tracking this material in Arctic rivers such as the Kolyma River in Siberia has proven challenging due to its high biodegradability. Here, we evaluate late summer abruptly thawed yedoma permafrost dissolved organic carbon (DOC) inputs from Duvannyi Yar. We implemented ultrahigh-resolution mass spectrometry alongside ramped pyrolysis oxidation (RPO) and isotopic analyses. These approaches offer insight into DOM chemical composition and DOC radiocarbon values of thermochemical components for a permafrost thaw stream, the Kolyma River, and their biodegraded counterparts (n = 4). The highly aliphatic molecular formula found in undegraded permafrost DOM contrasted with the comparatively aliphatic-poor formula of Kolyma River DOM, represented by an 8.9% and 2.6% relative abundance, respectively, suggesting minimal inputs of undegraded permafrost DOM in the river. RPO radiocarbon fractions of Kolyma River DOC exhibited no “hidden” aged component indicative of permafrost influence. Thermostability analyses suggested that there was limited biodegraded permafrost DOC in the Kolyma River, in part determined by the formation of high-activation energy (thermally stable) biodegradation components in permafrost DOM that were lacking in the Kolyma River. A mixing model based on thermostability and radiocarbon allowed us to estimate a maximum input of between 0.8% and 7.7% of this Pleistocene-aged permafrost to the Kolyma River DOC. Ultimately, our findings highlight that export of modern terrestrial DOC currently overwhelms any permafrost DOC inputs in the Kolyma River.
    Description: This work was funded by NSF grants ANT-1203885 and PLR-1500169 to R.G.M.S. The work was also supported by the National Science Foundation Division of Chemistry through DMR-1644779 and the State of Florida.
    Description: 2022-01-09
    Keywords: Permafrost ; Dissolved organic carbon ; Dissolved organic matter ; FT-ICR MS ; Ramped pyrolysis oxidation ; Arctic
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 2
    Publication Date: 2022-10-26
    Description: Author Posting. © American Geophysical Union, 2021. 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 35(4), (2021): e2020GB006895, https://doi.org/10.1029/2020GB006895.
    Description: The Amazon River drains a diverse tropical landscape greater than 6 million km2, culminating in the world's largest export of freshwater and dissolved constituents to the ocean. Here, we present dissolved organic carbon (DOC), organic and inorganic nitrogen (DON, DIN), orthophosphate (PO43−), and major and trace ion concentrations and fluxes from the Amazon River using 26 samples collected over three annual hydrographs. Concentrations and fluxes were predominantly controlled by the annual wet season flood pulse. Average DOC, DON, DIN, and PO43− fluxes (±1 s.d.) were 25.5 (±1.0), 1.14 (±0.05), 0.82 (±0.03), and 0.063 (±0.003) Tg yr−1, respectively. Chromophoric dissolved organic matter absorption (at 350 nm) was strongly correlated with DOC concentrations, resulting in a flux of 74.8 × 106 m−2 yr−1. DOC and DON concentrations positively correlated with discharge while nitrate + nitrite concentrations negatively correlated, suggesting mobilization and dilution responses, respectively. Ammonium, PO43−, and silica concentrations displayed chemostatic responses to discharge. Major and trace ion concentrations displayed clockwise hysteresis (except for chloride, sodium, and rubidium) and exhibited either dilution or chemostatic responses. The sources of weathered cations also displayed seasonality, with the highest proportion of carbonate- and silicate-derived cations occurring during peak and baseflow, respectively. Finally, our seasonally resolved weathering model resulted in an average CO2 consumption yield of (3.55 ± 0.11) × 105 mol CO2 km−2 yr−1. These results represent an updated and temporally refined quantification of dissolved fluxes that highlight the strong seasonality of export from the world's largest river and set a robust baseline against which to gauge future change.
    Description: This work was supported by a grant from the Harbourton Foundation to R. G. M. Spencer and R. M. Holmes. T. W. Drake was supported by ETH Zurich core funding to J. Six. R. G. M. Spencer was additionally supported by NSF OCE-1333157.
    Description: 2021-09-15
    Keywords: Amazon river ; Dissolved organic carbon ; Fluxes ; Weathering ; Geochemistry
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
    Publication Date: 2022-05-27
    Description: Author Posting. © American Geophysical Union, 2021. 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 35(6), (2021): e2021GB006938, https://doi.org/10.1029/2021GB006938.
    Description: As climate-driven El Niño Southern Oscillation (ENSO) events are projected to increase in frequency and severity, much attention has focused on impacts regarding ecosystem productivity and carbon balance in Amazonian rainforests, with comparatively little attention given to carbon dynamics in fluvial ecosystems. In this study, we compared the wet 2012 La Niña period to the following normal hydrologic period in the Amazon River. Elevated water flux during the La Niña period was accompanied by dilution of inorganic ion concentrations. Furthermore, the La Niña period exported 2.77 Tg C yr−1 more dissolved organic carbon (DOC) than the normal period, an increase greater than the annual amount of DOC exported by the Mississippi River. Using ultra-high-resolution mass spectrometry, we detected both intra- and interannual differences in dissolved organic matter (DOM) composition, revealing that DOM exported during the dry season and the normal period was more aliphatic, whereas compounds in the wet season and following the La Niña event were more aromatic, with ramifications for its environmental role. Furthermore, as this study has the highest temporal resolution DOM compositional data for the Amazon River to-date we showed that compounds were highly correlated to a 6-month lag in Pacific temperature and pressure anomalies, suggesting that ENSO events could impact DOM composition exported to the Atlantic Ocean. Therefore, as ENSO events increase in frequency and severity into the future it seems likely that there will be downstream consequences for the fate of Amazon Basin-derived DOM concurrent with lag periods as described here.
    Description: This work was partially supported by National Science Foundation grant OCE-1464396 to Robert G. M. Spencer and funding from the Harbourton Foundation to Robert G. M. Spencer, R. Max Holmes, and Bernhard Peucker-Ehrenbrink.
    Description: 2021-12-11
    Keywords: Amazon river ; carbon cycling ; dissolved organic carbon ; dissolved organic matter ; ENSO ; FT-ICR MS
    Repository Name: Woods Hole Open Access Server
    Type: Article
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