Fluvial organic carbon composition regulated by seasonal variability in lowland river migration and water discharge

Identifying drivers of seasonal variations in fluvial particulate organic carbon (POC) composition can aid sediment provenance and biogeochemical cycling studies. We evaluate seasonal changes in POC composition in the Río Bermejo, Argentina, a lowland river running ∼1,270 km without tributaries. Weekly POC concentration and isotopic composition from 2016 to 2018 show that during the wet season, increased lateral channel migration generates an influx of 13C-enriched and 14C-enriched floodplain-sourced material, overprinting the 13C-depleted and 14C-depleted headwater signature that is observed during the dry season. These findings demonstrate how channel morphodynamics can drive variability of POC composition in lowland rivers, and may modulate the composition of POC preserved in sedimentary archives

Particulate Organic Matter Mobilization and Transformation Along a Himalayan River Revealed by ESI‐FT‐ICR‐MS

Tracing pathways and transformations of particulate organic carbon from landscape sources to oceanic sinks is commonly done using the isotopic composition or biomarker content of particulate organic matter (POM). However, similarity of source characteristics and complex mixing in rivers often preclude a robust deconvolution of individual contributions. Moreover, these approaches are limited in detecting organic matter transformations. This impedes understanding of carbon cycling. Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FT‐ICR‐MS) can simultaneously identify many molecular formulas from mixtures of organic matter, and provide direct information on its compositional variability. Here, we investigate how FT‐ICR‐MS can give insight into POM dynamics on a landscape scale, focusing on the trans‐Himalayan Kali Gandaki River, Nepal. Using molecular information, we identify source tracers in the solvent extractable lipid fraction of riverine POM, finding up to 102 indicative molecular formulas for individual sources. Further, we assess molecular transformations of the lipid fraction of POM during its transfer from litter into topsoil, and onwards into the river. A large number of shared mass formulas and a well‐preserved isoprenoidal patterns suggest efficient incorporation of litter into topsoil. In contrast, we observe a selective loss of mass formulas and a preferential export of formulas with low double bond equivalents and a low nominal oxidation state of carbon after organic matter entrainment in the river. Our results demonstrate the potential of FT‐ICR‐MS for source‐to‐sink studies, allowing detailed organic matter source characterization and discrimination, and tracking of molecular transformations along organic matter pathways spanning different spatial and temporal scales.Plain Language Summary: The transfer of organic matter (OM) by rivers from landscape sources into the ocean followed by its burial in marine sediments is an important carbon sink. Therefore, OM is often traced along this journey using its isotopic or biomarker composition. But contributions of OM sources to river sediments can be difficult to estimate because of similar source characteristics, mixing of many sources and changes of the molecular composition along the way. Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FT‐ICR‐MS) is a novel method able to identify many molecular formulas from OM mixtures at once providing direct information about their molecular composition. Here, we investigate how FT‐ICR‐MS contributes to understanding the transport and transformation of particulate OM focusing on a Himalayan river in Nepal. We use the molecular information to identify tracers for individual OM sources in the landscape. We then assess molecular transformations during the transfer of litter into topsoil, and onwards into the river. Our data suggest efficient incorporation of litter into topsoil, but we observe a selective loss of molecular formulas upon entrainment of sources into the river. Our results reveal that FT‐ICR‐MS is useful for detailed source characterization and tracking of molecular transformations along OM pathways.Key Points: Organic matter sourcing and transformations in a Himalayan river studied by FT‐ICR‐MS measurements of solvent extractable lipids. Identification of up to 102 indicator mass formulas for different organic matter sources in the landscape using indicator species analysis. Mass formulas preserved during incorporation of litter into topsoil but selectively lost during entrainment of sources into the river.Helmholtz Impuls und VernetzungsfondGFZ expedition fundinghttp://doi.org/10.5880/GFZ.4.6.2022.00

Hg concentrations and stable isotope variations in tropical fish species of a gold-mining-impacted watershed in French Guiana

International audienc

Quantifying the impacts of artisanal gold mining on a tropical river system using mercury isotopes

International audienceTotal mercury (Hg) concentrations, speciation and isotopic composition were analyzed in soils and sediments along the Oyapock River (French Guiana), subjected to intense artisanal and small-scale gold-mining (ASGM). As a large part of these mining activities is illegal, amalgamation of gold with liquid Hg(0) is the main exploitation process. Further chemical analyses were performed along the same river, in bedrocks, waters, suspended matter, sediments and soils in both pristine and gold-mining areas. Physico-chemical parameters and Hg isotopic composition measured in the different matrices of the pristine area allowed us to trace the origin and fate of the natural Hg. We find that Hg in tropical topsoils preferentially originates from gaseous Hg(0) uptake by plants rather than from wet deposition. A strong negative mass independent fractionation (MIF) between topsoils and deeper horizons was attributed to pre-anthropogenic atmospheric Hg deposition with low MIF that leached to deeper horizons. Hg isotopic composition in pristine sediments confirmed that Hg in river sediments mainly originates from deep soil erosion and is subjected to aquatic photochemical reduction. Combining a Hg-isotope binary mixing model with a multiple linear regression based on physico-chemical parameters, we determined that the currently mined creek sediments are contaminated in Hg. This excess of Hg, which can represent more than half of the total Hg concentration, mainly originates from liqui

Paleosol-derived data used for the reconstruction of environmental conditions during the Holocene in the upper part of the Kali Gandaki valley, Central Nepal

This data publication contains the data sets of a study aiming to reconstruct environmental conditions during the Holocene in the upper part of the Kali Gandaki valley, Nepal. The data are for samples taken from paleosol sections in the Upper Mustang region (Menges et al. 2019). On these samples we measured the grain size distribution to gain information about the depositional processes, pollen data to reconstruct past vegetation, 14C isotopes in the humin fraction of organic matter for soil formation ages, and hydrogen isotopic composition on n-alkanes to reconstruct past hydrological conditions. This is complemented with optically stimulated luminescence data for additional depositional age information, surface water samples and modern soil samples to constrain modern hydrological conditions, and sediment concentration data to gain insights into erosion processes. The data was generated between 2013-02 and 2018-12. The data files are provided in Excel and tab-delimited text versions

Late Holocene Landscape Collapse of a Trans-Himalayan Dryland: Human Impact and Aridification

International audienceSoil degradation is a severe and growing threat to ecosystem services globally. Soil loss is often nonlinear, involving a rapid deterioration from a stable eco-geomorphic state once a tipping point is reached. Soil loss thresholds have been studied at plot scale, but for landscapes, quantitative constraints on the necessary and sufficient conditions for tipping points are rare. Here, we document a landscape-wide eco-geomorphic tipping point at the edge of the Tibetan Plateau and quantify its drivers and erosional consequences. We show that in the upper Kali Gandaki valley, Nepal, soil formation prevailed under wetter conditions during much of the Holocene. Our data suggest that after a period of human pressure and declining vegetation cover, a 20% reduction of relative humidity and precipitation below 200 mm/year halted soil formation after 1.6 ka and promoted widespread gullying and rapid soil loss, with irreversible consequences for ecosystem services

Suspended sediment collected from Puente La Valle (PLV, -25.655°S, -60.130°W) between 2016 - 2018

These data were collected from the Río Bermejo in northern Argentina. To determine the seasonal variability in the particulate organic carbon composition of exported river sediment, we collected weekly suspended sediment samples (March 2016 to March 2018) at the Puente Lavalle (PLV) monitoring site, ~870 river km downstream of the mountain front (-25.655°S, -60.130°W). Surface water samples were collected from a bridge using a river-rinsed bucket and were filtered through a 0.22 µm polyethersulfone membrane. Samples were stored on site at ambient temperatures for up to one year, transferred to Germany and subsequently stored at ~4°C until processing. Suspended sediment was rinsed from filters into pre-combusted glass evaporating dishes using ultra-pure (18.2 M) water, oven-dried at 40°C for >48 hr, and homogenized in an agate mortar without crushing. Geochemical and grain size analyses required 0.8 g sediment; for samples 0.8 g (Table S1). We split sediment samples into aliquots for grain size analysis via laser diffraction and geochemical analyses. Sediment particle size distributions were measured on ~0.2 g aliquots using a laser diffraction particle size analyzer (Retsch/Horiba LA-950V2). Aliquots for geochemical analyses were ground to <63 µm. The homogenized suspended sediment, bedrock, soil and leaf litter aliquots were further split for total nitrogen measurement (TN, wt%) and organic carbon analyses including total organic carbon (TOC, wt%), stable carbon isotope composition (δ13COC), and radiocarbon fraction modern (Fm). We decarbonated the aliquots for POC measurements using a liquid HCl leach following Galy et al., (2007). TOC and TN measurements were split between facilities at the German Research Centre for Geosciences (GFZ), Durham University, and University of Nevada Reno (UNR) using an elemental analyzer (EA). δ13COC was measured with a coupled EA-isotope ratio mass spectrometer (EA-IRMS). All isotopic compositions are reported using standard delta (δ) notation in per mil (‰) relative to Vienna PeeDee Belemnite (VPDB). Calibration and accuracy were monitored through analyses of in-house standards (Glutamic Acid, 40.82% C, 9.52% N at Durham; Boden3, HEKATECH at GFZ), which were calibrated against international standards (e.g., USGS 40, USGS 24, IAEA 600, IAEA CH3, IAEA CH7, IAEA N1, IAEA N2). Radiocarbon content was measured for a subset of 29 samples at ETH Zürich using a combined EA and accelerator mass spectrometer (EA-AMS) (Ruff et al. 2010; McIntyre et al., 2017). All 14C /12C ratios are reported as fraction modern (Fm, equivalent to F14C as defined by Reimer et al. (2004)) relative to 95% of the 14C activity of NBS Oxalic Acid II in 1950 (δ13COC = -17.8‰) and normalized to δ13COC = -25‰ of VPDB.\n\nThis geochemical dataset is supported by hydrologic measurements of daily water discharge at the El Colorado gauging station (river km 1086, SNIH, https://snih.hidricosargentina.gob.ar/) collected between 2016 and 2018

Overview of endmember samples collected along the Río Bermejo

To document distinct sources of particulate organic carbon (POC) to the Río Bermejo, we collected 15 soil and 13 leaf litter samples from the local floodplain, and 10 bedrock (predominantly outcroppings of fine-grained sedimentary bedrock) and 2 soil samples from the Río Bermejo headwaters. Leaf litter and soil were oven-dried at 40°C for >48 hours. We shredded leaf litter in an industrial blender, homogenized soil samples in an agate mortar and manually removed root and plant debris >1 cm, and pulverized bedrock samples to <63 µm

Seasonal variability of fluvial organic carbon composition between 2016-2018 in the Río Bermejo, Argentina

These data were collected from the Río Bermejo in northern Argentina. To determine the seasonal variability in the particulate organic carbon composition of exported river sediment, we collected weekly suspended sediment samples (March 2016 to March 2018) at the Puente Lavalle (PLV) monitoring site, ~870 river km downstream of the mountain front (-25.655°S, -60.130°W). Surface water samples were collected from a bridge using a river-rinsed bucket and were filtered through a 0.22 µm polyethersulfone membrane. Samples were stored on site at ambient temperatures for up to one year, transferred to Germany and subsequently stored at ~4°C until processing. To document distinct sources of particulate organic carbon (POC) to the Río Bermejo, we collected 15 soil and 13 leaf litter samples from the local floodplain, and 10 bedrock (predominantly outcroppings of fine-grained sedimentary bedrock) and 2 soil samples from the Río Bermejo headwaters. Suspended sediment was rinsed from filters into pre-combusted glass evaporating dishes using ultra-pure (18.2 M) water, oven-dried at 40°C for >48 hr, and homogenized in an agate mortar without crushing. Leaf litter and soil were oven-dried at 40°C for >48 hours. We shredded leaf litter in an industrial blender, homogenized soil samples in an agate mortar and manually removed root and plant debris >1 cm, and pulverized bedrock samples to 0.8 g (Table S1). We split sediment samples into aliquots for grain size analysis via laser diffraction and geochemical analyses. Sediment particle size distributions were measured on ~0.2 g aliquots using a laser diffraction particle size analyzer (Retsch/Horiba LA-950V2). Aliquots for geochemical analyses were ground to <63 µm. The homogenized suspended sediment, bedrock, soil and leaf litter aliquots were further split for total nitrogen measurement (TN, wt%) and organic carbon analyses including total organic carbon (TOC, wt%), stable carbon isotope composition (δ13COC), and radiocarbon fraction modern (Fm). We decarbonated the aliquots for POC measurements using a liquid HCl leach following Galy et al. (2007, doi:10.1111/j.1751-908X.2007.00864.x)). TOC and TN measurements were split between facilities at the German Research Centre for Geosciences (GFZ), Durham University, and University of Nevada Reno (UNR) using an elemental analyzer (EA). δ13COC was measured with a coupled EA-isotope ratio mass spectrometer (EA-IRMS). All isotopic compositions are reported using standard delta (δ) notation in per mil (‰) relative to Vienna PeeDee Belemnite (VPDB). Calibration and accuracy were monitored through analyses of in-house standards (Glutamic Acid, 40.82% C, 9.52% N at Durham; Boden3, HEKATECH at GFZ), which were calibrated against international standards (e.g., USGS 40, USGS 24, IAEA 600, IAEA CH3, IAEA CH7, IAEA N1, IAEA N2). Radiocarbon content was measured for a subset of 29 samples at ETH Zürich using a combined EA and accelerator mass spectrometer (EA-AMS) (Ruff et al. (2010, doi:10.1017/S003382220005637X); McIntyre et al. (2017, doi:10.1017/RDC.2016.68)). All 14C /12C ratios are reported as fraction modern (Fm, equivalent to F14C as defined by Reimer et al. (2004)) relative to 95% of the 14C activity of NBS Oxalic Acid II in 1950 (δ13COC = -17.8‰) and normalized to δ13COC = -25‰ of VPDB. This geochemical dataset is supported by hydrologic measurements of daily water discharge at the El Colorado gauging station (river km 1086, SNIH, https://snih.hidricosargentina.gob.ar/) collected between 2016 and 2018