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  • Dissolved organic matter  (3)
  • Alkalinity  (1)
  • Biomarkers  (1)
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  • 1
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2019. This is the author's version of the work. It is posted here by permission of Elsevier Ltd. for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 244 (2019): 216-228, doi:10.1016/j.gca.2018.10.012.
    Description: Mountain glaciers store dissolved organic carbon (DOC) that can be exported to river networks and subsequently respired to CO2. Despite this potential importance within the global carbon cycle, the seasonal variability and downstream transport of glacier-derived DOC in mountainous river basins remains largely unknown. To provide novel insight, here we present DOC concentrations and molecular-level dissolved organic matter (DOM) compositions from 22 nested, glaciated catchments (1.4 – 81.8 % glacier cover by area) in the Upper Ganges Basin, Western Himalaya over the course of the Indian summer monsoon (ISM) in 2014. Aliphatic and peptide-like compounds were abundant in glaciated headwaters but were overprinted by soil-derived phenolic, polyphenolic and condensed aromatic material as DOC concentrations increase moving downstream. Across the basin, DOC concentrations and soil-derived compound class contributions decreased sharply from pre- to post-ISM, implying increased relative contribution of glaciated headwater signals as the monsoon progresses. Incubation experiments further revealed a strong compositional control on the fraction of bioavailable DOC (BDOC), with glacier-derived DOC exhibiting the highest bioavailability. We hypothesize that short-term (i.e. in the coming decades) increases in glacier melt flux driven by climate change will further bias exported DOM toward an aliphatic-rich, bioavailable signal, especially during the ISM and post-ISM seasons. In contrast, eventual decreases in glacier melt flux due to mass loss will likely lead to more a soil-like DOM composition and lower bioavailability of exported DOC in the long term.
    Description: We thank Britta Voss (WHOI) for assisting with sample collection; Travis Drake (FSU), and Ekaterina Bulygina (Woods Hole Research Center) for laboratory assistance; and the NHMFL ICR user program (NSF-DMR-1157490) for aiding in data acquisition and analysis. This study was partly supported by NSF-DEB-1145932 to R.G.M.S. J.D.H. was partially supported by the NSF Graduate Research Fellowship Program under grant number 2012126152, with additional support in the form of travel grants awarded by the MIT Houghten Fund and NHMFL. All data used in this study are available in the Supporting Information Tables S1 and S2.
    Keywords: Dissolved organic matter ; Eco-hydrology ; Glaciers ; Himalaya ; Monsoon
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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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 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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  • 3
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2013. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 40 (2013): 511–516, doi:10.1002/grl.50160.
    Description: Seasonal variations in inorganic carbon chemistry and associated fluxes from the Congo River were investigated at Brazzaville-Kinshasa. Small seasonal variation in dissolved inorganic carbon (DIC) was found in contrast with discharge-correlated changes in pH, total alkalinity (TA), carbonate species, and dissolved organic carbon (DOC). DIC was almost always greater than TA due to the importance of CO2*, the sum of dissolved CO2 and carbonic acid, as a result of low pH. Organic acids in DOC contributed 11–61% of TA and had a strong titration effect on water pH and carbonate speciation. The CO2* and bicarbonate fluxes accounted for ~57% and 43% of the DIC flux, respectively. Congo River surface water released CO2 at a rate of ~109 mol m−2 yr−1. The basin-wide DIC yield was ~8.84 × 104 mol km−2 yr−1. The discharge normalized DIC flux to the ocean amounted to 3.11 × 1011 mol yr−1. The DOC titration effect on the inorganic carbon system may also be important on a global scale for regulating carbon fluxes in rivers.
    Description: This project was supported by a grant from the National Science Foundation for the Global Rivers Project (NSF 0851101).
    Description: 2013-08-14
    Keywords: Inorganic carbon ; Carbon dioxide ; Carbon fluxes ; pH ; Alkalinity ; Congo River
    Repository Name: Woods Hole Open Access Server
    Type: Article
    Format: application/pdf
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  • 4
    Publication Date: 2022-05-26
    Description: © The Author(s), 2017. 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 Chemical Geology 466 (2017): 454-465, doi:10.1016/j.chemgeo.2017.06.034.
    Description: We present dissolved organic carbon (DOC) concentrations, particulate organic matter (POM) composition (δ13C, δ15N, ∆14C, N/C), and particulate glycerol dialkyl glycerol tetraether (GDGT) distributions from a 34-month time-series near the mouth of the Congo River. An end-member mixing model using δ13C and N/C indicates that exported POM is consistently dominated by C3 rainforest soil sources, with increasing contribution from C3 vegetation and decreasing contribution from phytoplankton at high discharge. Large C4 inputs are never observed despite covering ≈ 13 % of the catchment. Low and variable ∆14C values during 2011 [annual mean = (-148 ± 82) ‰], when discharge from left-bank tributaries located in the southern hemisphere reached record lows, likely reflect a bias toward pre-aged POM derived from the Cuvette Congolaise swamp forest. In contrast, ∆14C values were stable near -50 ‰ between January and June 2013, when left-bank discharge was highest. We suggest that headwater POM is replaced and/or diluted by C3 vegetation and pre-aged soils during transit through the Cuvette Congolaise, whereas left-bank tributaries export significantly less pre-aged material. GDGT distributions provide further evidence for seasonal and inter-annual variability in soil provenance. The cyclization of branched tetraethers and the GDGT-0 to crenarchaeol ratio are positively correlated with discharge (r ≥ 0.70; p-value ≤ 4.3×10-5) due to the incorporation of swamp-forest soils when discharge from right-bank tributaries located in the northern hemisphere is high. Both metrics reach record lows during 2013, supporting our interpretation of increased left-bank contribution at this time. We conclude that hydrologic variability is a major control of POM provenance in the Congo River Basin and that tropical wetlands can be a significant POM source despite their small geographic coverage.
    Description: J.D.H. was supported by the NSF Graduate Research Fellowship Program under grant number 2012126152; E.S. was supported by the DFG Research Center/Cluster of Excellence “The Ocean in the Earth System” at MARUM – Center for Environmental Sciences; V.V.G. was partly supported by the US National Science Foundation, grants OCE-0851015 and OCE-0928582; R.G.M.S. was partly supported by the US National Science Foundation, grants OCE-0851101, OCE-1333157, and OCE-1464396; and T.I.E. was partly supported by the Swiss National Science Foundation (SNF Grant No. 200021_140850).
    Keywords: Biomarkers ; Congo River ; GDGTs ; Particulate Organic Matter ; Radiocarbon
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 5
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2014. 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 119 (2014): 687–702, doi:10.1002/2013JG002442.
    Description: Dissolved organic carbon (DOC) and inorganic carbon (DIC, pCO2), lignin biomarkers, and theoptical properties of dissolved organic matter (DOM) were measured in a gradient of streams and rivers within the Congo Basin, with the aim of examining how vegetation cover and hydrology influences the composition and concentration of fluvial carbon (C). Three sampling campaigns (February 2010, November 2010, and August 2011) spanning 56 sites are compared by subbasin watershed land cover type (savannah, tropical forest, and swamp) and hydrologic regime (high, intermediate, and low). Land cover properties predominately controlled the amount and quality of DOC, chromophoric DOM (CDOM) and lignin phenol concentrations (∑8) exported in streams and rivers throughout the Congo Basin. Higher DIC concentrations and changing DOM composition (lower molecular weight, less aromatic C) during periods of low hydrologic flow indicated shifting rapid overland supply pathways in wet conditions to deeper groundwater inputs during drier periods. Lower DOC concentrations in forest and swamp subbasins were apparent with increasing catchment area, indicating enhanced DOC loss with extended water residence time. Surface water pCO2 in savannah and tropical forest catchments ranged between 2,600 and 11,922 µatm, with swamp regions exhibiting extremely high pCO2 (10,598–15,802 µatm), highlighting their potential as significant pathways for water-air efflux. Our data suggest that the quantity and quality of DOM exported to streams and rivers are largely driven by terrestrial ecosystem structure and that anthropogenic land use or climate change may impact fluvial C composition and reactivity, with ramifications for regional C budgets and future climate scenarios.
    Description: This work was supported by the National Science Foundation as part of the ETBC Collaborative Research: Controls on the Flux, Age, and Composition of Terrestrial Organic Carbon Exported by Rivers to the Ocean (0851101 and 0851015).
    Description: 2014-10-30
    Keywords: Dissolved organic matter ; Lignin ; CDOM ; pCO2 ; Aquatic ; Hydrology
    Repository Name: Woods Hole Open Access Server
    Type: Article
    Format: text/richtext
    Format: application/vnd.ms-excel
    Format: application/pdf
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