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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Dissolved Inorganic Carbon-Accumulating Complexes from Autotrophic Bacteria from Extreme Environments

To facilitate the synthesis of biomass from CO 2 , autotrophic organisms use a variety of mechanisms to increase intracellular DIC concentrations. A novel type of multi-subunit complex has recently been described, which has been shown to generate measurably elevated intracellular DIC concentrations in three species of bacteria, raising the question of whether these complexes share this capability across the 17 phyla of Bacteria and Archaea where they are found.

carbon fixation↗
DOE OSTI2024

A global database of dissolved organic matter (DOM) concentration measurements in coastal waters (CoastDOM v1)

Abstract. Measurements of dissolved organic carbon (DOC), nitrogen (DON), and phosphorus (DOP) concentrations are used to characterize the dissolved organic matter (DOM) pool and are important components of biogeochemical cycling in the coastal ocean. Here, we present the first edition of a global database (CoastDOM v1; available at https://doi.org/10.1594/PANGAEA.964012, Lønborg et al., 2023) compiling previously published and unpublished measurements of DOC, DON, and DOP in coastal waters. These data are complemented by hydrographic data such as temperature and salinity and, to the extent possible, other biogeochemical variables (e.g. chlorophyll a, inorganic nutrients) and the inorganic carbon system (e.g. dissolved inorganic carbon and total alkalinity). Overall, CoastDOM v1 includes observations of concentrations from all continents. However, most data were collected in the Northern Hemisphere, with a clear gap in DOM measurements from the Southern Hemisphere. The data included were collected from 1978 to 2022 and consist of 62 338 data points for DOC, 20 356 for DON, and 13 533 for DOP. The number of measurements decreases progressively in the sequence DOC > DON > DOP, reflecting both differences in the maturity of the analytical methods and the greater focus on carbon cycling by the aquatic science community. The global database shows that the average DOC concentration in coastal waters (average ± standard deviation (SD): 182±314 µmol C L−1; median: 103 µmol C L−1) is 13-fold higher than the average coastal DON concentration (13.6±30.4 µmol N L−1; median: 8.0 µmol N L−1), which is itself 39-fold higher than the average coastal DOP concentration (0.34±1.11 µmol P L−1; median: 0.18 µmol P L−1). This dataset will be useful for identifying global spatial and temporal patterns in DOM and will help facilitate the reuse of DOC, DON, and DOP data in studies aimed at better characterizing local biogeochemical processes; closing nutrient budgets; estimating carbon, nitrogen, and phosphorous pools; and establishing a baseline for modelling future changes in coastal waters.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Composition and Flux of Dissolved and Particulate Carbon and Nitrogen in the Lower Tocantins River

The Tocantins River contributes ~5 % of the total flux of water to the Amazon River plume in the Atlantic Ocean. Here, we evaluate monthly variability in the composition and abundance of carbon, nitrogen, and suspended sediment in the lower reaches of the Tocantins River from 2014-2016. Dissolved organic carbon (DOC) concentrations generally increased during periods of high discharge and are ~1.5 times lower than average concentrations at the mouth of the Amazon River. Dissolved inorganic carbon (DIC) similarly increased during periods of high discharge. Total dissolved nitrogen (TDN) and individual nitrogen species followed a similar temporal pattern, increasing during high water. $\text{NO}^-_3$ predominated the dissolved inorganic nitrogen (DIN) pool, followed by $\text{NH}_4^+$, and $\text{NO}_2^-$ , characteristic of environments with a relatively low anthropogenic impact. Dissolved fractions represented 92 % of the total carbon exported and 78 % of the total nitrogen exported. The suspended particulate sediment flux was 2.72 x 10 6 t yr -1 , with fine suspended sediment (FSS) dominating (71.3 %). Concentrations of carbon relative to nitrogen indicate a primarily terrigenous source of organic matter and CO 2 derived from in situ respiration of this material during the rainy season and a primarily algal/bacterial source of organic matter during the dry season. Considering past estimates of dissolved carbon and nitrogen fluxes from the Amazon River to the Atlantic Ocean, the Tocantins River contributes 3 and 3.7 % to total fluxes to the Amazon River plume region, respectively. While this contribution is relatively small, it may be influenced by future changes to the basin’s land use and hydrology.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

SPRUCE Outflow Chemistry Data for Experimental Plots Beginning in 2016

This data set includes the chemistry of outflow waters in the SPRUCE experiment plots located in the S1 bog of the USDA Forest Service Marcell Experimental Forest (MEF) in northern Minnesota, 40 km north of Grand Rapids. These data are post-treatment data from the warming and elevated carbon dioxide (CO2) treatments associated with the SPRUCE experiment. There are ten experimental plots in SPRUCE: five temperature treatments (+0, +2.25, +4.5, +6.75, +9°C) at ambient CO2, and the same five temperature treatments at elevated CO2 (+500 ppm). Sample collection and analyses started in March of 2016 and will continue for the duration of the experiment. Samples were analyzed for pH, specific conductivity, anion concentrations (chloride, sulfate), cation concentrations (calcium, potassium, magnesium, sodium, aluminum, iron, manganese, silicon, strontium), nutrient concentrations (ammonium, nitrate, soluble reactive phosphorus, total nitrogen, total phosphorus), and total organic carbon (TOC) concentrations. Subsets of the samples have been analyzed for natural-abundance stable isotopes of water (δ18O-H2O and δD-H2O), dissolved carbon dioxide (δ13C-CO2), and dissolved methane (δ13C-CH4), and concentrations of total mercury (Thg), methylmercury (MeHg), ferrous iron (Fe2+), ferric iron (Fe3+), dissolved inorganic carbon (DIC), and dissolved methane (CH4).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Integrating Tide‐Driven Wetland Soil Redox and Biogeochemical Interactions Into a Land Surface Model

Abstract Redox processes, aqueous and solid‐phase chemistry, and pH dynamics are key drivers of subsurface biogeochemical cycling and methanogenesis in terrestrial and wetland ecosystems but are typically not included in terrestrial carbon cycle models. These omissions may introduce errors when simulating systems where redox interactions and pH fluctuations are important, such as wetlands where saturation of soils can produce anoxic conditions and coastal systems where sulfate inputs from seawater can influence biogeochemistry. Integrating cycling of redox‐sensitive elements could therefore allow models to better represent key elements of carbon cycling and greenhouse gas production. We describe a model framework that couples the Energy Exascale Earth System Model (E3SM) Land Model (ELM) with PFLOTRAN biogeochemistry, allowing geochemical processes and redox interactions to be integrated with land surface model simulations. We implemented a reaction network including aerobic decomposition, fermentation, sulfate reduction, sulfide oxidation, methanogenesis, and methanotrophy as well as pH dynamics along with iron oxide and iron sulfide mineral precipitation and dissolution. We simulated biogeochemical cycling in tidal wetlands subject to either saltwater or freshwater inputs driven by tidal hydrological dynamics. In simulations with saltwater tidal inputs, sulfate reduction led to accumulation of sulfide, higher dissolved inorganic carbon concentrations, lower dissolved organic carbon concentrations, and lower methane emissions than simulations with freshwater tidal inputs. Model simulations compared well with measured porewater concentrations and surface gas emissions from coastal wetlands in the Northeastern United States. These results demonstrate how simulating geochemical reaction networks can improve land surface model simulations of subsurface biogeochemistry and carbon cycling.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Long-Term 13 C Uptake by 12 C-Enriched Calcite

Knowledge of the exchange of carbon isotopes between dissolved inorganic carbon and calcite minerals is of long-standing importance for the interpretation of sedimentary paleoclimate records and 14 C transport in the geosphere. To assess the mechanism and rates of carbon isotope exchange, we equilibrated 12 C-pure synthetic calcite particles in water, first in a glovebox and then in contact with atmospheric P CO 2 and 13 C/ 12 C ratio, at two different temperatures. Cavity ring-down infrared spectroscopy δ 13 C measurements of the solid revealed sustained 13C incorporation for over a period of 500 days (21 °C) and 125 days (50 °C). We developed a quantitative model for recrystallization and isotope exchange, assuming that the interfacial free energy provides a thermodynamic driving force for the growth of larger particles at the expense of smaller ones. Furthermore, this Ostwald ripening model did not reproduce the kinetics of 13C uptake and required greater coarsening than observed. Rather, the data were best explained by a mechanism involving surface exchange and solid-phase diffusion of 13C into the particles with an inferred effective diffusion constant at 21 °C of about 10 –25 m 2 /s. Although this work cannot rule out the possibility that structural or chemical aspects of the synthetic particles enabled faster 13 C uptake than could be observed in natural systems, this study adds to the body of the recent work, suggesting that fast exchange processes are possible, likely through grain boundaries and other defects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Adsorption of Neodymium, Dysprosium, and Ytterbium to Goethite under Varying Aqueous Chemistry Conditions

The adsorption of rare earth elements (REEs) to iron oxides can regulate the mobility of REEs in the environment and is heavily influenced by water chemistry. This study utilized batch experiments to examine the adsorption of Nd, Dy, and Yb to goethite under varying pH, electrolyte (type and concentration), and concentrations of dissolved inorganic carbon and citrate. REE adsorption was strongly influenced by pH, with an increase from essentially no adsorption at pH 3.0 to nearly complete adsorption at pH 6.5 and higher. Citrate enhanced the adsorption of REEs at low pH (<5.0), likely by forming goethite-REE-citrate ternary surface complexes. However, citrate inhibited the adsorption of REEs at higher pH (>5.0) by forming aqueous REE-citrate complexes. Ionic strength had a small influence on REE adsorption, and the presence of dissolved inorganic carbon had no discernible effect. Equilibrium adsorption was interpreted with a triple-layer surface complexation model (SCM). The selection of surface complexation reactions was guided by extended X-ray absorption fine structure spectra. An SCM with a single bidentate inner-sphere surface complexation reaction for Nd and two inner-sphere surface complexation reactions (one monodentate and one bidentate reaction) for Dy and Yb effectively simulated adsorption across a broad range of conditions in the absence of citrate. Accounting for the effects of citrate on REE adsorption required the addition of up to two ternary REE-citrate-goethite surface complexes. The SCM can enable predictions of REE transport in subsurface environments that have goethite as an important adsorbent mineral. Furthermore, this predictive capability could contribute to identifying potential REE sources and facilitating efficient extraction of REEs.

58 GEOSCIENCES↗
DOE OSTI2024

Adsorption of neodymium, dysprosium, and ytterbium to goethite under varying aqueous chemistry conditions [dataset]

The adsorption of rare earth elements (REEs) to iron oxides can regulate the mobility of REEs in the environment and is heavily influenced by water chemistry. This study utilized batch experiments to examine the adsorption of Nd, Dy, and Yb to goethite under varying pH, electrolyte (type and concentration), and concentrations of dissolved inorganic carbon and citrate. REE adsorption was strongly influenced by pH, with an increase from essentially no adsorption at pH 3.0 to nearly complete adsorption at pH 6.5 and higher. Citrate enhanced the adsorption of REEs at low pH (< 5.0), likely by forming goethite-REE-citrate ternary surface complexes. However, citrate inhibited the adsorption of REEs at higher pH (> 5.0) by forming aqueous REE-citrate complexes. Ionic strength had a small influence on REE adsorption, and the presence of dissolved inorganic carbon had no discernible effect. Equilibrium adsorption was interpreted with a triple layer surface complexation model (SCM). The selection of surface complexation reactions was guided by extended X-ray absorption fine structure spectra. A SCM with a single bidentate inner-sphere surface complexation reaction for Nd and two inner-sphere surface complexation reactions (one monodentate and one bidentate reaction) for Dy and Yb effectively simulated adsorption across a broad range of conditions in the absence of citrate. Accounting for the effects of citrate on REE adsorption required the addition of up to two ternary REE-citrate-goethite surface complexes. The SCM can enable predictions of REE transport in subsurface environments that have goethite as an important adsorbent mineral. This predictive capability could contribute to identifying potential REE sources and facilitating efficient extraction of REEs.

58 GEOSCIENCES↗
DOE OSTI2023

Carbon Outgassing in the Antarctic Circumpolar Current Is Supported by Ekman Transport From the Sea Ice Zone in an Observation‐Based Seasonal Mixed‐Layer Budget

Despite its importance for the global cycling of carbon, there are still large gaps in our understanding of the processes driving annual and seasonal carbon fluxes in the high-latitude Southern Ocean. This is due in part to a historical paucity of observations in this remote, turbulent, and seasonally ice-covered region. Here, we use autonomous biogeochemical float data spanning 6 full seasonal cycles and with circumpolar coverage of the Southern Ocean, complemented by atmospheric reanalysis, to construct a monthly climatology of the mixed layer budget of dissolved inorganic carbon (DIC). We investigate the processes that determine the annual mean and seasonal cycle of DIC fluxes in two different zones of the Southern Ocean—the Sea Ice Zone (SIZ) and Antarctic Southern Zone (ASZ). We find that, annually, mixing with carbon-rich waters at the base of the mixed layer supplies DIC which is, in the ASZ, either used for net biological production or outgassed to the atmosphere. In contrast, in the SIZ, where carbon outgassing and the biological pump are weaker, the surplus of DIC is instead advected northward to the ASZ. In other words, carbon outgassing in the southern Antarctic Circumpolar Current (ACC), which has been attributed to remineralized carbon from deep water upwelled in the ACC, is also due to the wind-driven transport of DIC from the SIZ. These results stem from the first observation-based carbon budget of the circumpolar Southern Ocean and thus provide a useful benchmark to evaluate climate models, which have significant biases in this region.

Sauvé, Jade↗
DOE OSTI2020

Tracking natural CO 2 migration through a sandstone aquifer using Sr, U and C isotopes: Chimayó, New Mexico, USA

The geochemical and isotopic characteristics of groundwaters in Chimayó, New Mexico, reflect processes that affect water quality in the Tesuque Aquifer, which overlies a leaking natural CO 2 source in a structurally complex region. In this study, select isotopes (δ 13 C, 87 Sr/ 86 Sr, 234 U/ 238 U) are applied to groundwaters to better understand CO 2 transport mechanisms and related water-rock interactions that impact Chimayó groundwater. Carbon stable isotope ratios of dissolved inorganic carbon (DIC; δ 13 CDIC = -15.10‰ to 4.50‰) identify a distinct source of upward-migrating CO 2 that interacts with the groundwater. Additionally, groundwater 87 Sr/ 86 Sr compositions (0.7098 to 0.7154) reflect intrusion of varying amounts of saline water associated with the high CO 2 source, while 234 U/ 238 U ratios corroborate presence of deep groundwater and suggest impacts from distinctive natural uranium sources are affecting groundwater. Previous work proposed two CO 2 transport mechanisms at the site: (1) dissolved in deep brine that underlies the aquifer and (2) in the gas phase; this study uses isotope mixing models to identify wells that are affected by these CO 2 transport mechanisms and demonstrates that both transport mechanisms are associated with impaired groundwaters. Overall, this study demonstrates that applying multiple isotope systems (δ 13 CDIC, 87 Sr/ 86 Sr, 234 U/ 238 U) is a dynamic tool for identifying and measuring the impact of CO 2 leakage from a sequestration site.

58 GEOSCIENCES↗
DOE OSTI2020

Improved CO 2 utilization efficiency using membrane carbonation in outdoor raceways

Membrane carbonation, the delivery of CO 2 by diffusion through non-porous hollow fiber membranes, was successfully integrated into outdoor raceways (5.6 m 2 , 900 L) and operated continuously for up to 45 days. Biomass productivity associated with membrane carbonation was similar to using traditional sparging, but the average carbon utilization efficiencies for membrane carbonation was 3-fold higher than for sparging when 100% CO 2 was delivered to both systems. Here, when the pH setpoint was 8.5, growth on ammonium bicarbonate using membrane carbonation achieved a carbon utilization efficiency of 106 ± 45% due to uptake of some carbon from bicarbonate. Using nitrate as the N source had a 78 ± 55% carbon utilization efficiency, due to dissolved inorganic carbon accumulation as the medium alkalinity increased. Lowering the pH setpoint to 8.0 created a carbon-rich environment that decreased the carbon utilization efficiency to 51 ± 27% due to CO 2 off-gassing, but it still was 3-fold higher than with sparging.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation

Abstract The direct utilization of dissolved inorganic carbon in seawater for CO 2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO 2 reduction (CO 2 R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO 2 (aq) (CO 2 dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO 2 (aq) as a reactant generated in situ by acidification of HCO 3 - flows continuously from BiVO 4 photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO 4 PEC CO 2 R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale.

Liu, Bin↗
DOE OSTI2022

Alkaline cation enrichment and water electrolysis to provide CO 2 mineralization and global-scale carbon management

Provided herein are methods of removing carbon dioxide from an aqueous stream or gaseous stream by: contacting the gaseous stream comprising carbon dioxide, when present, with an aqueous solution comprising ions capable of forming an insoluble carbonate salt; contacting the aqueous solution comprising carbon dioxide with an electroactive mesh that induces its alkalinization thereby forcing the precipitation of a carbonate solid from the solution and thereby the removal of dissolved inorganic carbon by electrolysis; and removing the precipitated carbonate solids from the solution, or the surface of the mesh where they may deposit. Also provided herein are flow-through electrolytic reactors comprising an intake device in fluid connection with a rotating cylinder comprising an electroactive mesh, and a scraping device and/or liquid-spray based device for separating a solid from the mesh surface.

Sant, Gaurav↗
DOE OSTI2024

Surface water geochemistry along St. Louis River Estuary (Duluth/Superior, MN/WI)

This dataset is aimed at understanding changes in surface water chemistry associated with urbanization in the Great Lakes region. Surface water chemistry including cations, anions, organic and inorganic carbon, and nitrogen were collected from six locations along St. Louis River – a freshwater estuary entering Lake Superior (Duluth/Superior, MN/WI). The Duluth/Superior, MN/WI metropolitan area is the largest port on the United States side of Lake Superior. Samples were collected near different land uses every two weeks from late July 2023 to the onset of ice cover in November 2023. Water samples were analyzed using In-Situ AquaTroll 500 Multiparameter Sonde with Ammonium Ion Selective Electrode and Chlorophyll-a sensor (unfiltered), METTLER TOLEDO FiveEasy Plus FP20 and METTLER TOLEDO LE407 probe (unfiltered); HACH DR300 Pocket Colorimeter Iron FerroVer (filtered 0.22 μm in field); Shimadzu TOC-L Total Organic Carbon Analyzer with TNM-L Total Nitrogen Unit (filtered 0.22 μm in field); Agilent 8900 triple quadrupole ICP-MS (ICP-QQQ) (filtered 0.22 μm in field); and Dionex ICS-6000 HPIC System (filtered 0.22 μm in field).The data package is comprised of 5 files. dd.csv contains the description of columns in Geochemistry_LSNERR_water.csv and Sampling_sites.csv. flmd.csv contains descriptions of each file in the dataset. README.txt contains description of the dataset structure and file content. Geochemistry_LSNERR_water.csv contains geochemistry data for six sampling locations along the St. Louis River. Sampling_sites.csv contains latitude and longitude coordinates for each of the six sampling site locations along the St. Louis River.This data has not been previously published.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Functional plasticity of HCO 3 – uptake and CO 2 fixation in Cupriavidus necator H16

Despite its prominence, the ability to engineer Cupriavidus necator H16 for inorganic carbon uptake and fixation is underexplored. We tested the roles of endogenous and heterologous genes on C. necator inorganic carbon metabolism. Deletion of β-carbonic anhydrase can had the most deleterious effect on C. necator autotrophic growth. Replacement of this native uptake system with several classes of dissolved inorganic carbon (DIC) transporters from Cyanobacteria and chemolithoautotrophic bacteria recovered autotrophic growth and supported higher cell densities compared to wild-type (WT) C. necator in batch culture. Strains expressing Halothiobacillus neopolitanus DAB2 (hnDAB2) and diverse rubisco homologs grew in CO 2 similarly to the wild-type strain. Our experiments suggest that the primary role of carbonic anhydrase during autotrophic growth is to support anaplerotic metabolism, and an array of DIC transporters can complement this function. This work demonstrates flexibility in HCO 3 - uptake and CO 2 fixation in C. necator, providing new pathways for CO 2 -based biomanufacturing.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

Quantitative stable isotope probing (qSIP)-informed metagenomics identifies viruses infecting chemoautotrophs

Aquatic environments absorb ~2.5 gigatonnes of atmospheric carbon each year1, more than the carbon stored in the atmosphere, soils, and all biomass combined. Primary producers transform this dissolved inorganic carbon into biomass that can subsequently flow into other trophic levels, or be released back into the environment through viral lysis. While there is substantial knowledge about the diversity and activity of viruses infecting photoautotrophic primary producers and the ecosystem impact, little is known about viruses infecting chemoautotrophs, representing a gap in our understanding of key processes driving microbial carbon cycling. Here, we combine metagenomics with quantitative 12/13C stable isotopic probing (qSIP) mesocosm experiments in a marine-derived meromictic pond to quantify population-specific isotopic enrichment, identify key chemoautotrophic primary producers, and virus-host dynamics. Isotopically enriched carbon is tracked from the genomes of chemoautotrophs to putative viruses, showing that active populations of hydrogen/sulfur-oxidizing chemoautotrophs (Thiomicrorhabdus, Hydrogenovibrio, Sulfurimonas, Sulfurovum) are targeted by viruses. This work provides the foundation for revealing the diversity and activity of viruses infecting globally-widespread chemoautotrophs. Our study sheds light on trophic interactions that impact microbial carbon cycling in aphotic environments and builds toward biogeochemical models that incorporate viral impacts on chemoautotrophic microbial communities.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

A New Framework for the Attribution of Air‐Sea CO 2 Exchange

Abstract The air‐sea transfer of carbon dioxide can be viewed as a dynamic system through which atmospheric and oceanic processes push surface waters away from thermodynamic equilibrium, while diffusive gas transfer pulls them back toward local equilibrium. These push/pull processes drive significant sub‐seasonal, seasonal, and interannual variability in air‐sea carbon fluxes, the quantification of which is critical both for diagnosing the ocean response to fossil fuel emissions and for attempts to mitigate anthropogenic climate disruption through intentional modification of surface ocean biogeochemistry. In this study, we present a new approach for attributing air‐sea carbon fluxes to specific mechanisms. The new framework is first applied to a two‐box ocean nutrient and carbon cycle model as an illustrative example. Next, outputs from a regional eddy‐resolving model of the Southern Ocean are analyzed. The roles of multiple physical and biogeochemical processes are identified. The decomposition of the seasonal air‐sea carbon flux shows the dominant role of biological carbon pumps that are partially compensated by the transport convergence. Finally, the framework is used to diagnose the response to mesoscale iron and alkalinity release, explicitly quantifying transport feedback and eventual impacts on net air‐sea carbon flux. Ocean carbon transport has divergent influences between iron and alkalinity release, due to opposing near‐surface gradients of dissolved inorganic carbon. We suggest that our attribution framework may be a useful analytical technique for monitoring natural ocean carbon fluxes and quantifying the impacts of human intervention on the ocean carbon cycle.

Ito, Takamitsu [School of Earth and Atmospheric Sc↗
DOE OSTI2026

Model‐Based Interpretation of Solute Exports and Carbon Partitioning During Shale Weathering in a Mountainous Hillslope

The weathering of sedimentary rocks in high-elevation catchments influences freshwater quality and the global carbon cycle. While individual biogeochemical mechanisms involved in this process are relatively well understood, quantifying their contributions to solute export and carbon fluxes under natural, transient conditions remains challenging. Here, we implement a numerical multidimensional and multiphase model to simulate coupled hydrological and biogeochemical processes in a shale-underlain, snow-dominated hillslope in the Rocky Mountains, Colorado. The model captures the dynamic interplay between soil respiration, mineral weathering, and climate-driven hydrological forcing, reproducing observed soil CO 2 dynamics, groundwater chemistry, and subsurface flow. Our results reveal that seasonal snowmelt enhances carbonate weathering by promoting the infiltration of CO 2 -rich water to depth, while pyrite oxidation is primarily sensitive to low water saturation that facilitates O 2 diffusion through the regolith. Topography modulates the spatial distribution of shale weathering, as steeper slopes enhance lateral drainage, favoring the delivery of reactants to greater depths. While shale weathering at our site acts as a transient carbon sink, with silicates and carbonates buffering acidity and promoting atmospheric CO 2 consumption (1% of soil-derived CO 2 ), the exported dissolved inorganic carbon is predominantly geogenic (∼73%). Consequently, when accounting for long-term marine carbonate precipitation. The current weathering regime represents a net source of carbon to the atmosphere. The oxidation of pyrite and petrogenic organic carbon together release approximately 0.9 mol·m −2 ·yr −1 of CO 2 . Our findings highlight the role of topography, hydroclimate, and the coupling between acid-base reactions in shaping the carbon balance and the solute exports in mountainous critical zones.

carbon cycling↗