skip to main content

Title: Machine learning deciphers CO<sub>2</sub> sequestration and subsurface flowpaths from stream chemistry
Abstract. Endmember mixing analysis (EMMA) is often used by hydrogeochemiststo interpret the sources of stream solutes, but variations in streamconcentrations and discharges remain difficult to explain. We discoveredthat machine learning can be used to highlight patterns in stream chemistrythat reveal information about sources of solutes and subsurface groundwaterflowpaths. The investigation has implications, in turn, for the balance ofCO2 in the atmosphere. For example, CO2-driven weathering ofsilicate minerals removes carbon from the atmosphere over ∼106-year timescales. Weathering of another common mineral, pyrite, releases sulfuricacid that in turn causes dissolution of carbonates. In that process,however, CO2 is released instead of sequestered from the atmosphere. Thus, understanding long-term global CO2 sequestration by weatheringrequires quantification of CO2- versus H2SO4-drivenreactions. Most researchers estimate such weathering fluxes from streamchemistry, but interpreting the reactant minerals and acids dissolved in streams has been fraught with difficulty. We apply a machine-learningtechnique to EMMA in three watersheds to determine the extent of mineraldissolution by each acid, without pre-defining the endmembers. The resultsshow that the watersheds continuously or intermittently sequester CO2, but the extent of CO2 drawdown is diminished in areas heavily affectedby acid rain. Prior to applying the new algorithm, CO2 drawdown wasoverestimated. The new technique, which elucidates the importance more » ofdifferent subsurface flowpaths and long-timescale changes in the watersheds,should have utility as a new EMMA for investigating water resourcesworldwide. « less
Authors:
; ; ;
Award ID(s):
1331726 1639150
Publication Date:
NSF-PAR ID:
10313541
Journal Name:
Hydrology and Earth System Sciences
Volume:
25
Issue:
6
ISSN:
1607-7938
Sponsoring Org:
National Science Foundation
More Like this
  1. Soil biota generate CO2 that can vertically export to the atmosphere, and dissolved organic and inorganic carbon (DOC and DIC) that can laterally export to streams and accelerate weathering. These processes are regulated by external hydroclimate forcing and internal structures (permeability distribution), the relative influences of which are rarely studied. Understanding these interactions is essential a hydrological extremes intensify in the future. Here we explore the question: How and to what extent do hydrological and permeability distribution conditions regulate soil carbon transformations and chemical weathering? We address the questions using a hillslope reactive transport model constrained by data from the Fitch Forest (Kansas, United States). Numerical experiments were used to mimic hydrological extremes and variable shallow-versus-deep permeability contrasts. Results demonstrate that under dry conditions (0.08 mm/day), long water transit times led to more mineralization of organic carbon (OC) into inorganic carbon (IC) form (>98\%). Of the IC produced, ~ 75\% was emitted upward as CO2 gas and ~ 25\% was exported laterally as DIC into the stream. Wet conditions (8.0 mm/day) resulted in less mineralization (~88\%), more DOC production (~12\%), and more lateral fluxes of IC (~50\% of produced IC). Carbonate precipitated under dry conditions and dissolved under wet conditionsmore »as the fast flow rapidly droves the reaction to disequilibrium. The results depict a conceptual hillslope model that prompts four hypotheses for our community to test. H1: Droughts enhance carbon mineralization and vertical upward carbon fluxes, whereas large hydrological events such as storms and flooding enhance subsurface vertical connectivity, reduce transit times, and promote lateral export. H2: The role of weathering as a net carbon sink or source to the atmosphere depends on the interaction between hydrologic flows and lithology: transition from droughts to storms can shift carbonate from a carbon sink (mineral precipitation) to carbon source (dissolution). H3: Permeability contrasts regulate the lateral flow partitioning via shallow flow paths versus deeper groundwater though this alter reaction rates negligibly. H4: Stream chemistry reflect flow paths and can potentially quantify water transit times: solutes enriched in shallow soils have a younger water signature; solutes abundant at depth carry older water signature.« less
  2. null (Ed.)
    Abstract. Carbonate weathering is essential in regulating atmosphericCO2 and carbon cycle at the century timescale. Plant roots accelerateweathering by elevating soil CO2 via respiration. It however remainspoorly understood how and how much rooting characteristics (e.g., depth anddensity distribution) modify flow paths and weathering. We address thisknowledge gap using field data from and reactive transport numericalexperiments at the Konza Prairie Biological Station (Konza), Kansas (USA), asite where woody encroachment into grasslands is surmised to deepen roots. Results indicate that deepening roots can enhance weathering in two ways.First, deepening roots can control thermodynamic limits of carbonatedissolution by regulating how much CO2 transports vertical downward tothe deeper carbonate-rich zone. The base-case data and model from Konzareveal that concentrations of Ca and dissolved inorganic carbon (DIC) areregulated by soil pCO2 driven by the seasonal soil respiration. Thisrelationship can be encapsulated in equations derived in this workdescribing the dependence of Ca and DIC on temperature and soil CO2. The relationship can explain spring water Ca and DIC concentrations from multiple carbonate-dominated catchments. Second, numericalexperiments show that roots control weathering rates by regulating recharge(or vertical water fluxes) into the deeper carbonate zone and exportreaction products at dissolution equilibrium. The numerical experimentsexplored the potential effects of partitioningmore »40 % of infiltrated waterto depth in woodlands compared to 5 % in grasslands. Soil CO2 datasuggest relatively similar soil CO2distribution over depth, which in woodlands and grasslands leads only to 1 % to∼ 12 % difference inweathering rates if flow partitioning was kept the same between the two landcovers. In contrast, deepening roots can enhance weathering by ∼ 17 % to200 % as infiltration rates increased from 3.7 × 10−2 to 3.7 m/a. Weathering rates in these cases however are more than an order of magnitude higher than a case without roots atall, underscoring the essential role of roots in general. Numericalexperiments also indicate that weathering fronts in woodlands propagated> 2 times deeper compared to grasslands after 300 years at aninfiltration rate of 0.37 m/a. These differences in weathering fronts areultimately caused by the differences in the contact times of CO2-charged water with carbonate in the deep subsurface. Within the limitation of modeling exercises, these data and numerical experiments prompt the hypothesis that (1) deepening roots in woodlands can enhance carbonate weathering by promotingrecharge and CO2–carbonate contact in the deepsubsurface and (2) the hydrological impacts of rooting characteristics canbe more influential than those of soil CO2 distribution in modulatingweathering rates. We call for colocated characterizations of roots,subsurface structure, and soil CO2 levels, as well as their linkage to waterand water chemistry. These measurements will be essential to illuminatefeedback mechanisms of land cover changes, chemical weathering, globalcarbon cycle, and climate.« less
  3. Abstract. The western Arctic Ocean, including its shelves and coastal habitats, has become a focus in ocean acidification research over the past decade as thecolder waters of the region and the reduction of sea ice appear to promote the uptake of excess atmospheric CO2. Due to seasonal sea icecoverage, high-frequency monitoring of pH or other carbonate chemistry parameters is typically limited to infrequent ship-based transects duringice-free summers. This approach has failed to capture year-round nearshore carbonate chemistry dynamics which is modulated by biological metabolismin response to abundant allochthonous organic matter to the narrow shelf of the Beaufort Sea and adjacent regions. The coastline of the Beaufort Seacomprises a series of lagoons that account for > 50 % of the land–sea interface. The lagoon ecosystems are novel features that cycle between“open” and “closed” phases (i.e., ice-free and ice-covered, respectively). In this study, we collected high-frequency pH, salinity,temperature, and photosynthetically active radiation (PAR) measurements in association with the Beaufort Lagoon Ecosystems – Long Term Ecological Research program – for an entire calendar yearin Kaktovik Lagoon, Alaska, USA, capturing two open-water phases and one closed phase. Hourly pH variability during the open-water phases are someof the fastest rates reported, exceeding 0.4 units. Baseline pH varied substantially between themore »open phase in 2018 and open phase in 2019 from ∼ 7.85to 8.05, respectively, despite similar hourly rates of change. Salinity–pH relationships were mixed during all three phases, displaying nocorrelation in the 2018 open phase, a negative correlation in the 2018/19 closed phase, and a positive correlation during the 2019 open phase. The high frequency of pH variabilitycould partially be explained by photosynthesis–respiration cycles as correlation coefficients between daily average pH and PAR were 0.46 and 0.64for 2018 and 2019 open phases, respectively. The estimated annual daily average CO2 efflux (from sea to atmosphere) was5.9 ± 19.3 mmolm-2d-1, which is converse to the negative influx of CO2 estimated for the coastal Beaufort Seadespite exhibiting extreme variability. Considering the geomorphic differences such as depth and enclosure in Beaufort Sea lagoons, furtherinvestigation is needed to assess whether there are periods of the open phase in which lagoons are sources of carbon to the atmosphere, potentiallyoffsetting the predicted sink capacity of the greater Beaufort Sea.« less
  4. International Ocean Discovery Program (IODP) Expedition 382, Iceberg Alley and Subantarctic Ice and Ocean Dynamics, investigated the long-term climate history of Antarctica, seeking to understand how polar ice sheets responded to changes in insolation and atmospheric CO2 in the past and how ice sheet evolution influenced global sea level and vice versa. Five sites (U1534–U1538) were drilled east of the Drake Passage: two sites at 53.2°S at the northern edge of the Scotia Sea and three sites at 57.4°–59.4°S in the southern Scotia Sea. We recovered continuously deposited late Neogene sediment to reconstruct the past history and variability in Antarctic Ice Sheet (AIS) mass loss and associated changes in oceanic and atmospheric circulation. The sites from the southern Scotia Sea (Sites U1536–U1538) will be used to study the Neogene flux of icebergs through “Iceberg Alley,” the main pathway along which icebergs calved from the margin of the AIS travel as they move equatorward into the warmer waters of the Antarctic Circumpolar Current (ACC). In particular, sediments from this area will allow us to assess the magnitude of iceberg flux during key times of AIS evolution, including the following: • The middle Miocene glacial intensification of the East Antarctic Ice Sheet,more »• The mid-Pliocene warm period, • The late Pliocene glacial expansion of the West Antarctic Ice Sheet, • The mid-Pleistocene transition (MPT), and • The “warm interglacials” and glacial terminations of the last 800 ky. We will use the geochemical provenance of iceberg-rafted detritus and other glacially eroded material to determine regional sources of AIS mass loss. We will also address interhemispheric phasing of ice sheet growth and decay, study the distribution and history of land-based versus marine-based ice sheets around the continent over time, and explore the links between AIS variability and global sea level. By comparing north–south variations across the Scotia Sea between the Pirie Basin (Site U1538) and the Dove Basin (Sites U1536 and U1537), Expedition 382 will also deliver critical information on how climate changes in the Southern Ocean affect ocean circulation through the Drake Passage, meridional overturning in the region, water mass production, ocean–atmosphere CO2 transfer by wind-induced upwelling, sea ice variability, bottom water outflow from the Weddell Sea, Antarctic weathering inputs, and changes in oceanic and atmospheric fronts in the vicinity of the ACC. Comparing changes in dust proxy records between the Scotia Sea and Antarctic ice cores will also provide a detailed reconstruction of changes in the Southern Hemisphere westerlies on millennial and orbital timescales for the last 800 ky. Extending the ocean dust record beyond the last 800 ky will help to evaluate dust-climate couplings since the Pliocene, the potential role of dust in iron fertilization and atmospheric CO2 drawdown during glacials, and whether dust input to Antarctica played a role in the MPT. The principal scientific objective of Subantarctic Front Sites U1534 and U1535 at the northern limit of the Scotia Sea is to reconstruct and understand how ocean circulation and intermediate water formation responds to changes in climate with a special focus on the connectivity between the Atlantic and Pacific basins, the “cold water route.” The Subantarctic Front contourite drift, deposited between 400 and 2000 m water depth on the northern flank of an east–west trending trough off the Chilean continental shelf, is ideally situated to monitor millennial- to orbital-scale variability in the export of Antarctic Intermediate Water beneath the Subantarctic Front. During Expedition 382, we recovered continuously deposited sediments from this drift spanning the late Pleistocene (from ~0.78 Ma to recent) and from the late Pliocene (~3.1–2.6 Ma). These sites are expected to yield a wide array of paleoceanographic records that can be used to interpret past changes in the density structure of the Atlantic sector of the Southern Ocean, track migrations of the Subantarctic Front, and give insights into the role and evolution of the cold water route over significant climate episodes, including the following: • The most recent warm interglacials of the late Pleistocene and • The intensification of Northern Hemisphere glaciation.« less
  5. International Ocean Discovery Program Expedition 382, Iceberg Alley and Subantarctic Ice and Ocean Dynamics, investigated the long-term climate history of Antarctica, seeking to understand how polar ice sheets responded to changes in insolation and atmospheric CO2 in the past and how ice sheet evolution influenced global sea level and vice versa. Five sites (U1534–U1538) were drilled east of the Drake Passage: two sites at 53.2°S at the northern edge of the Scotia Sea and three sites at 57.4°–59.4°S in the southern Scotia Sea. We recovered continuously deposited late Neogene sediments to reconstruct the past history and variability in Antarctic Ice Sheet (AIS) mass loss and associated changes in oceanic and atmospheric circulation. The sites from the southern Scotia Sea (Sites U1536–U1538) will be used to study the Neogene flux of icebergs through “Iceberg Alley,” the main pathway along which icebergs calved from the margin of the AIS travel as they move equatorward into the warmer waters of the Antarctic Circumpolar Current (ACC). In particular, sediments from this area will allow us to assess the magnitude of iceberg flux during key times of AIS evolution, including the following: • The middle Miocene glacial intensification of the East Antarctic Ice Sheet, •more »The mid-Pliocene warm period, • The late Pliocene glacial expansion of the West Antarctic Ice Sheet, • The mid-Pleistocene transition (MPT), and • The “warm interglacials” and glacial terminations of the last 800 ky. We will use the geochemical provenance of iceberg-rafted detritus and other glacially eroded material to determine regional sources of AIS mass loss. We will also address interhemispheric phasing of ice sheet growth and decay, study the distribution and history of land-based versus marine-based ice sheets around the continent over time, and explore the links between AIS variability and global sea level. By comparing north–south variations across the Scotia Sea between the Pirie Basin (Site U1538) and the Dove Basin (Sites U1536 and U1537), Expedition 382 will also deliver critical information on how climate changes in the Southern Ocean affect ocean circulation through the Drake Passage, meridional overturning in the region, water mass production, ocean–atmosphere CO2 transfer by wind-induced upwelling, sea ice variability, bottom water outflow from the Weddell Sea, Antarctic weathering inputs, and changes in oceanic and atmospheric fronts in the vicinity of the ACC. Comparing changes in dust proxy records between the Scotia Sea and Antarctic ice cores will also provide a detailed reconstruction of changes in the Southern Hemisphere westerlies on millennial and orbital timescales for the last 800 ky. Extending the ocean dust record beyond the last 800 ky will help to evaluate dust-climate couplings since the Pliocene, the potential role of dust in iron fertilization and atmospheric CO2 drawdown during glacials, and whether dust input to Antarctica played a role in the MPT. The principal scientific objective of Subantarctic Front Sites U1534 and U1535 at the northern limit of the Scotia Sea is to reconstruct and understand how intermediate water formation in the southwest Atlantic responds to changes in connectivity between the Atlantic and Pacific basins, the “cold water route.” The Subantarctic Front contourite drift, deposited between 400 and 2000 m water depth on the northern flank of an east–west trending trough off the Chilean continental shelf, is ideally situated to monitor millennial- to orbital-scale variability in the export of Antarctic Intermediate Water beneath the Subantarctic Front. During Expedition 382, we recovered continuously deposited sediments from this drift spanning the late Pleistocene (from ~0.78 Ma to recent) and from the late Pliocene (~3.1–2.6 Ma). These sites are expected to yield a wide array of paleoceanographic records that can be used to interpret past changes in the density structure of the Atlantic sector of the Southern Ocean, track migrations of the Subantarctic Front, and give insights into the role and evolution of the cold water route over significant climate episodes, including the following: • The most recent warm interglacials of the late Pleistocene and • The intensification of Northern Hemisphere glaciation.« less