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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Effects of Interactions Between Produced Formation Fluid and Rock Matrix on Pore Structure of Caney Shale, Southern Oklahoma

ABSTRACT: Rock-fluid interactions change properties of shales during exploitation. To investigate effects of rock-fluid interactions on pore structure of shales matrix after hydraulic fracturing, powder samples from two late Mississippian Caney Shale cores in the Ardmore Basin, southern Oklahoma, were used to react with formation produced fluid from the field in the batch reactor analysis. X-ray diffraction for mineralogy and Low-pressure nitrogen adsorption isotherms for pore structure were measured for original, after-7days, and after-30days samples. Results show that the samples consist mainly of quartz, followed by clay minerals, carbonates, and feldspar. The pore sizes of micropore (<2 nm) and mesopore (2-50 nm) increase 14%-233% due to dissolution of pyrite, feldspar, and carbonates after 7 days. Due to the transformation from smectite to illite and the increase of pore size, the specific surface area (SSA) decreases after 7-days interactions. After 30-days interactions, the micropore volume slightly increases and the mesopore and macropore volume decreases. Due to the decrease of pore size, the SSA of 30-days reacted samples increases correspondingly and is lower (for the clay-rich sample) or higher (for the calcareous sample) than that of the unreacted samples. Findings improve our understanding of dynamic alteration of shale properties during production. 1. INTRODUCTION Energy demand will continuously grow owing to the increasing global population as well as energy consumption (EIA, 2023). On the other hand, shale gas and oil reshaped the energy market in the United States, enabling the United States to become a net-export of natural gas country in 2017 (EIA, 2023). However, shale reservoirs are challenging tight formations that are still poorly understood in the extraction and production of hydrocarbons (Ross and Bustin, 2009; Curtis et al., 2012; Xiong et al., 2015, 2021a; Li Y. et al., 2016; Gong et al., 2019a; Benge et al., 2021; Awejori et al., 2022; Huang et al., 2022). One of the most challenging topics is the rock-fluid interactions post hydraulic fracturing and its subsequent impacts on the pore structures of fractured formation matrix.

Xiong, Fengyang↗
NASA NTRS1999

Experimental Studies of Brines and Evaporites as Applied to Mars: Initial Results from 1998-1999 Runs

We are performing laboratory experiments to determine the concentrations and rates of dissolution of ions that could occur in closed, juvenile groundwater systems on Mars. Our approach is to incubate unaltered Mars-analog minerals in initially pure liquid water in contact with a Mars gas mixture for one year. At exponentially increasing time intervals, aliquots of the solutions at three different temperatures are extracted and analyzed using standard terrestrial laboratory geochemical techniques. Ultimately, our experiments will produce Mars analog brines which will be freeze dried to create evaporites. The physical and chemical properties of these evaporites will be compared with spacecraft remote sensing and in situ compositional and physical data. Additional information is contained in the original extended abstract.

Moore, J. M.↗
NASA NTRS1982

A non-catastrophist explanation for the iridium anomaly at the Cretaceous/Tertiary boundary

The iridium (Ir) anomaly at the Cretaceous/Tertiary (C/T) boundary can be explained by dissolution of normal pelagic limestones producing an insoluble clay residue containing Ir-rich meteoritic material. Further concentration of Ir and other trace metals in the clay can be explained by deposition under reducing conditions. Clay-mineral analyses indicate that the boundary clay is similar to locally derived clays in the limestones above and below the boundary, and contains no detectable exotic components. This supports a terrestrial origin for the boundary clay. The genesis of the boundary clay is attributed to changes in ocean chemistry (pH and oxygenation), leading to an interval of widespread dissolution of carbonate sequences in the oceans, and culminating in the development of submarine pyritic hardgrounds and a disconformity of global extent.

Rampino, M. R.↗
DOE OSTI2024

Geochemical-hydromechanical couplings during water-serpentinized harzburgite interactions at 20° C and 30 bars

Interaction of groundwater with the serpentinized harzburgites of the upper mantle plays an important role in the geologic carbon cycle and serpentinization processes. Here, in this study, an intact serpentinized harzburgite with more than 60% lizardite from the Semail ophiolite in Oman was reacted with water at near neutral pH and low PCO 2 to observe its dissolution behavior and reaction path within the CaO-MgO-SiO 2 -CO 2 -H 2 O system at 20 °C and 30 bars. In the experiment, mass (i.e. H 2 O, ions) transfer is by diffusion and the selected temperature and pressure conditions mimic water-rock interactions at the shallow portions of most ultramafic rock hosted aquifers. Equilibrium activity-activity diagrams and thermodynamic data were used to compare the experimentally determined reaction path with the theoretical stability boundaries for minerals involved to investigate the evolution of bulk chemical composition, mineralogy, and water composition. The experiments demonstrated that (i) the water-rock interactions increased the pH of the aqueous phase from 5.9 to 7.5 over a period of 18 weeks; (ii) the dissolution of lizardite, orthopyroxene (enstatite), and clinopyroxene (diopside and augite) increased the concentration of Mg, Ca, and Si in the aqueous phase; (iii) the dissolution was incongruent with respect to Mg and Si, favoring Si release at pH > 6 due to (a) breaking of more reactive cation‑oxygen bonds that is consistent with the stoichiometry of magnesium for proton exchange reaction which favors a surface that is enriched in Mg at basic conditions, and (b) preferential dissolution of clinopyroxene Mg 1.30 Ca 0.52 Fe 0.06 Si 2 O 6 ; (iv) the aqueous phase was undersaturated with respect to carbonate (e.g. calcite, magnesite, and hydromagnesite) and hydrous (e.g. lizardite, chrysotile, brucite, and talc) minerals; (v) the bulk chemical composition and mineralogy of the intact serpentinized harzburgite matrix did not change; (vi) the thermodynamic data can successfully predict water-intact serpentinized harzburgite behavior if the water chemical composition can be constrained; and (vii) no detectable macroscopic form of damage (e.g. microcracks forming as a result of differential stress fields due to changes in volume during chemical reaction) was observed.

Carbonation↗
NASA NTRS2007

Linking Home Plate and Algonquin Class Rocks through Microtextural Analysis: Evidence for Hydrovolcanism in the Inner Basin of Columbia Hills, Gusev Crater

Examining the his-tory of a rock as the summed history of its constituent grains is a proven and powerful strategy that has been used on Earth to maximize the information that can be gleaned from limited samples. Grain size, sorting, roundness, and texture can be observed at the handlens scale, and may reveal clues to transport regime (e.g. fluvial, glacial, eolian) and transport distance. Diagenetic minerals may be of a form and textural context to allow identification, and to point to dominant diagenetic processes (e.g. evaporitic concentration, intermittent dissolution, early vs. late diagenetic emplacement). Handlens scale features of volcaniclastic particles may be diagnostic of primary vs recycled (by surface processes) grains and may provide information about eruptive patterns and processes. When the study site is truly remote, such as Mars, and when there are severe limitations on sample return or sample analysis with other methods, examination at the hand lens scale becomes critical both for extracting a maximum of information, and for best utilizing finite analytical capabilities.

Mittlefehldt, David W.↗
NASA NTRS2014

Experimental Alteration of Basalt to Support Interpretation of Remote Sensing and In Situ Meausrements from Mars

Major occurrences of hydrous alteration minerals on Mars have been found in Noachian impact craters formed in basaltic targets and detected using visible/near infrared (VNIR) spectroscopy. Until recently phyllosilicates were detected only in craters in the southern hemisphere [1, 2]. However, it has been reported that at least nine craters in the northern plains apparently excavated thick layers of lava and sediment to expose phyllosilicates [3] as well. The MER (Mars Exploration Rovers) rovers previously reported results of in situ measurement indicating the presence of alteration minerals on Mars [4,5] and it was recently reported that the Mars Curiosity rover has detected alteration phases in situ at Yellowknife Bay in Gale crater as well [6,7]. An important discovery for Mars geochronology is that the Chemistry and Mineralogy (CheMin) x-ray diffraction (XRD) instrument on Curiosity detected phyllosilicates indicating that phyllosilicate formation on Mars extended beyond the Noachian Epoch [8]. These discoveries indicate that Mars was globally altered by water in the past but does not constrain formation conditions for alteration phase occurrences, which have important implications for the evolution of the surface and the biological potential on Mars. Understanding the alteration assemblages produced by a range of conditions is vital for the interpretation of phyllosilicate spectral signatures as well as in situ measurements and to decipher the environment and evolution of early Mars. The martian surface has been intensely altered by meteorite impacts whose effects include brecciation and melting of target materials as well as the initiation of hydrothermal circulation in a hydrous target [9,10,11,12]. Impact effects may facilitate aqueous alteration of a basaltic target because the rate of silicate dissolution is a function of the degree of crystallinity, surface area, and temperature. The resultant alteration mineralogies from shocked basaltic target material are a function of the original mineral assemblage in the parent rocks, the chemistry of fluids that interacted with the rocks, and physico-chemical conditions (pH, temperatures, and pressure) during the time of mineral formation. Understanding the alteration assemblages produced by a range of conditions is vital for the interpretation of phyllosilicate spectral signatures and to decipher the environment and evolution of early Mars, and especially for identifying habitable niches in which life could be initiated and sustained. No experimentally controlled and well characterized analog materials that simulate martian shock metamorphism and alteration conditions currently exist for calibrating either remote sensing or in situ measurements of Mars. A series of experiments was initiated to assess the effects of systematic changes in the physico-chemical conditions on Mars analog materials thereby providing samples to ground-truth Mars remote sensing observations from CRISM (Compact Reconnaissance Imaging Spectrometer for Mars) and in situ measurements from Opportunity's Mössbauer and Curiosity's CHEMIN (Chemistry and Mineralogy X-Ray Diffraction/XRay Fluorescence) instruments. Results of initial experimental runs as analysed by SEM-EDS (Secondary Electron Microscopy -Energy Dispersive Spectroscopy) and X-ray Diffraction (XRD) analysis are reported here and lay the foundation for comparison with shocked and altered samples that will be characterized in the next phase of this work.

Bell, M. S.↗
DOE OSTI2024

Iron dissolution from Patagonian dust in the Southern Ocean: under present and future conditions

Although the input of desert dust as a key source of trace metals in the Southern Ocean (SO) has been previously studied, the dissolution process of metals in surface waters, particularly iron (Fe), remain poorly understood. Given the crucial role of Fe in primary production and the biological carbon pump in the SO, we focused on experimental estimations of Fe dissolution from Patagonian dust, the primary natural dust source in the SO. Our study considered both current and projected future conditions, encompassing sea-surface warming, acidification, increased photosynthetically active radiation, and doubled dust inputs. Through controlled laboratory experiments using filtered SO seawater, conducted over 7 days, we assessed changes in particulate Fe (pFe) concentrations, Fe redox speciation (Fe(II)/Fe(III)), and in the mineralogy of Fe-bearing dust in abiotic condition. The predominant minerals in the dust included quartz and aluminosilicates, with silicon (Si), aluminum (Al), and Fe as the major elements. No significant alterations in the mineralogy and the elemental composition of the dust were recorded during the dissolution experiments, neither under present nor under projected future conditions. The particulate Fe(II)/Fe(III) ratio remained consistently at 0.25 during the experiments, unaffected by changed conditions. Consequently, changes in environmental conditions in the SO would therefore not significantly alter the mineralogy and redox speciation of pFe in the Patagonian dust. On the contrary, pFe exhibited a dissolution rate of 3.8% and 1.6% per day under present and future conditions, respectively. The environmental changes anticipated for 2100 in the SO will likely to result in a decrease in the dissolution rate of pFe. Thus, even though a doubling of dust input by 2100 is anticipated, it will unlikely provide significantly more dissolved Fe (dFe) in seawater in the SO. Consequently, the future intensification of Patagonian dust inputs may not alleviate the Fe limitation in the SO.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1994

A comparison of iron extraction methods for the determination of degree of pyritisation and the recognition of iron-limited pyrite formation

Measurements of degree of pyritisation require an estimate of sediment iron which is capable of reaction with dissolved sulphide to form pyrite, either directly or indirectly via iron monosulphide precursors. Three dissolution techniques (buffered dithionite, cold 1 M HCl, boiling 12 M HCl) were examined for their capacity to extract iron from a variety of iron minerals, and iron-bearing sediments, as a function of different extraction times and different grain sizes. All the iron oxides studied are quantitatively extracted by dithionite and boiling HCl (but not by cold HCl). Both HCl techniques extract more iron from silicates than does dithionite but probably about the same amounts as are potentially capable of sulphidation. Modern sediment studies indicate that most sedimentary pyrite is formed rapidly from iron oxides, with smaller amounts formed more slowly from iron silicates (if sufficient geologic time is available). It is therefore recommended that the degree of pyritisation be defined with respect to the dithionite-extractable (mainly iron oxide) pool and/or the boiling HCl-extractable pool (which includes some silicate iron) for the recognition of iron-limited pyritisation.

NASA Discipline Exobiology↗
NASA NTRS2005

Hematite Spherules in Basaltic Tephra Altered Under Aqueous, Acid-Sulfate Conditions on Mauna Kea Volcano, Hawaii: Possible Clues for the Occurrence of Hematite-Rich Spherules in the Burns Formation at Meridiani Planum, Mars

Iron-rich spherules (>90% Fe2O3 from electron microprobe analyses) approx.10-100 microns in diameter are found within sulfate-rich rocks formed by aqueous, acid-sulfate alteration of basaltic tephra on Mauna Kea volcano, Hawaii. Although some spherules are nearly pure Fe, most have two concentric compositional zones, with the core having a higher Fe/Al ratio than the rim. Oxide totals less than 100% (93-99%) suggest structural H2O and/or /OH. The transmission Moessbauer spectrum of a spherule-rich separate is dominated by a hematite (alpha-Fe2O3) sextet whose peaks are skewed toward zero velocity. Skewing is consistent with Al(3+) for Fe(3+) substitution and structural H2O and/or /OH. The grey color of the spherules implies specular hematite. Whole-rock powder X-ray diffraction spectra are dominated by peaks from smectite and the hydroxy sulfate mineral natroalunite as alteration products and plagioclase feldspar that was present in the precursor basaltic tephra. Whether spherule formation proceeded directly from basaltic material in one event (dissolution of basaltic material and precipitation of hematite spherules) or whether spherule formation required more than one event (formation of Fe-bearing sulfate rock and subsequent hydrolysis to hematite) is not currently constrained. By analogy, a formation pathway for the hematite spherules in sulfate-rich outcrops at Meridiani Planum on Mars (the Burns formation) is aqueous alteration of basaltic precursor material under acid-sulfate conditions. Although hydrothermal conditions are present on Mauna Kea, such conditions may not be required for spherule formation on Mars if the time interval for hydrolysis at lower temperatures is sufficiently long.

Morris, R. V.↗
DOE OSTI2024

Roles of kaolinite-oil-gas molecular interactions in hydrogen storage within depleted reservoirs

Hydrogen is a clean alternative to fossil fuels, emitting only water vapor during combustion. In a future hydrogen economy, large-scale storage will be an important component of the supply chain. Due to its low volumetric density, conventional surface storage methods are inadequate. Underground hydrogen storage (UHS) offers a viable solution, enabling the storage of millions of cubic meters. Among potential geological sites, including salt caverns, aquifers, and depleted gas reservoirs, depleted oil reservoirs show promise. Studying hydrogen interactions with residual oil and reservoir minerals is vital for understanding the properties of hydrogen and the reservoir post-injection. In this work, we employed molecular dynamics simulations to gain molecular-level insights into these interactions. We investigated hydrogen dissolution in oil, adsorption at kaolinite/oil interfaces, the role of CO 2 as a cushion gas, and the influence of kaolinite’s hydrophobicity on H 2 behavior. The main findings include: (1) hydrogen dissolves more in oil than in water, (2) the introduction of CO 2 suppresses hydrogen dissolution in oil and reduces the interfacial tension (IFT) between oil and gas, (3) CO 2 decreases H 2 partitioning near kaolinite surfaces due to its strong affinity for the hydrophilic gibbsite surface of kaolinite, and (4) CO 2 is more effective than H 2 in reducing IFT between kaolinite and the oil–gas mixture. These findings emphasize the effectiveness of CO 2 as a cushion gas and the important role of clay hydrophobicity in UHS, providing insights that are challenging to obtain experimentally.

08 HYDROGEN↗
DOE OSTI2026

Desorption of Phosphate from Iron-Bearing Soil Minerals by a Plant Secondary Metabolite

In soils, phosphorus readily adsorbs to the surfaces of ubiquitous iron (oxyhydr)oxide minerals, rendering it less accessible to plants and microorganisms. Plants have a number of strategies to access iron, among them the secretion of redox-active metabolites from their roots. Although these strategies likely increase the bioavailability of surface-adsorbed phosphorus through reductive dissolution, their effect on phosphorus cycling has not yet been investigated. We tested the ability of fraxetin, a coumarin-type redox-active metabolite produced by the model plant Arabidopsis thaliana and other dicotyledon plant species, to reductively solubilize phosphate from the surface of ferrihydrite. Our findings show that, at low and neutral pH, fraxetin increased aqueous phosphate concentrations under both oxic and anoxic conditions; at high pH, it was only effective in anoxic experiments. Additionally, a combination of liquid chromatography–mass spectrometry and spectroscopic methods demonstrated substantial fraxetin adsorption to the mineral surface but showed that iron reduction did not alter the mineral structure or change the nature of the chemical environment of the phosphorus atom over short time scales. These results provide evidence that the secretion of redox-active metabolites from roots is likely to be an effective phosphorus acquisition tactic in iron-rich soils.

36 MATERIALS SCIENCE↗
NASA NTRS2015

Survival of Organic Materials in Ancient Cryovolcanically-Produced Halite Crystals

Spectroscopic evidence supports the presence of Mg-Na-K salts derived from cryovolcanism on the surface of Europa. Halite (NaCl) is effective at very long-term preservation of organic phases and structures. Collection of salt crystals from Europan plumes would provide solid inclusions of organics, potentially also biomaterials, all suitable for analysis. Two thermally-metamorphosed ordinary chondrite regolith breccias (Monahans 1998 (H5) and Zag (H3-6)) contain fluid and solid inclusion-bearing halite crystals, dated to approximately 4.5 billion years, and thus the trapped aqueous fluids and solids are at least as old. Heating/freezing studies of the aqueous fluid inclusions in these halites demonstrated that they were trapped near 25 degrees Centigrade, and their continued presence in the halite grains requires that their incorporation into the H chondrite asteroid occurred after that body's metamorphism ended, since heating would have dessicated the halite. O and H isotopes of the trapped fluids are consistent with mixing of asteroidal and cometary water. Cryovolcanic Origin of the Halite: We hypothesize that these meteoritic halites derive from ancient cryovolcanism based on the following points. (1) Salts crystals are observed as products of current cryovolcanism on Enceladus. (2) In-situ spacecraft analysis of some of the icy grains associated with the Enceladus salt found minor organic or siliceous components, including methane, also found in the Monahans halite. (3) Cryovolcanic fluids are observed to be in chemical disequilibrium, reflecting incomplete reactions between interior volatiles and rocky materials. The coexistence of N2 and HCN in Enceladus' cryovolcanic fluids requires that the plume consists of a mixture of materials whose sources experienced different degrees of aqueous processing, including primordial material trapped in ice that has not been in contact with liquid water. The observed mineral assemblage within the Monahans and Zag halites is also far from equilibrium. Cryovolcanoes on Ceres are a potential source of our halite, however the processes that form halite should also be operating within Europa. Dissolution of Monahans halite grains has revealed a remarkable variety of organics, which dominate the population of solid inclusions. Thermal alteration of this macromolecular carbon (measured by Raman spectroscopy) shows remarkable diversity. We have identified highly-condensed aromatics, diamond, carbonates and chloromethane. Light organic compounds like methane tend to be water soluble and require cold formation temperatures at high hydrogen fugacity - i.e. require water ice. Another indication that these halites have not been heated is that light organics readily volatilize or aromaticize into PAHs. We are currently analyzing the organics by Raman and C-XANES, and measuring the content and exploring the potential chirality of amino acids in the halite. Implications for Europa Plumes: Organic materials and structures erupted by a Europa cryovolcano should be similarly preserved within halite, and other salts, which will be a convenient form for capture and analysis, since halite will serve to encapsulate and protect the organics from spacecraft contamination. Also, being transparent at many wavelengths halite will permit analysis by spacecraft-mounted spectroscopic techniques. In addition, halite is readily dissolved, permitting further analysis of entrained organics.

Zolensky, M.↗
NASA NTRS1999

Calcium Solubility In Zeolite Synthetic-Apatite Mixtures

Life support systems at a lunar or martian outpost will require the ability to produce food growing in 1) treated lunar or martian regolith; 2) a synthetic soil, or 3) some combination of both. Zeoponic soil, composed of NH4 (-) and K-exchanged clinoptilolite (Cp) and synthetic apatite (Ap), can provide slow-release fertilization via dissolution and ion-exchange. Equilibrium studies indicate that KNH4, P, and Mg are available to plants at sufficient levels, however, Ca is deficient. Ca availability can be increased by adding a second Ca-bearing mineral: calcite (Cal); dolomite (Dol); or wollastonite (Wol). Additions of Cal, Dol, and Wol systematically change the concentrations of Ca and P in solution. Cal has the greatest effect, Dol the least, and Wol is intermediate.

Beiersdorfer, R.↗
DOE OSTI2024

Silicate coprecipitation reduces green rust crystal size and limits dissolution-precipitation during air oxidation

Green rusts (GR) are mixed-valence iron (Fe) hydroxides which form in reducing redox environments like riparian and wetland soils and shallow groundwater. In these environments, silicon (Si) can influence Fe oxides’ chemical and physical properties but its role in GR formation and subsequent oxidative transformation have not been studied starting at initial nucleation. Green rust sulfate [GR(SO 4 )] and green rust carbonate [GR(CO 3 )] were both coprecipitated from salts by base titration in increasing % mol Si (0, 1, 10, and 50). The minerals were characterized before and after rapid (24 h) aqueous air-oxidation by x-ray diffraction (XRD), scanning electron microscopy (SEM), Fe extended x-ray absorption fine structure spectroscopy (EXAFS), and N 2 -BET surface area. Results showed that only GR(SO4) or GR(CO3) was formed at every tested Si concentration. Increasing % mol Si caused decreased plate size and increased surface area in GR(CO3) but not GR(SO4). GR plate basal thickness was not changed at any condition indicating a lack of Si interlayering. Air oxidation of GR(SO4) at all % mol Si contents transformed by dissolution and reprecipitation into lepidocrocite and goethite, favoring ferrihydrite with higher % Si content. Air oxidation of GR(CO3) transformed into magnetite and goethite but increasing Si caused GR to oxidize while retaining its hexagonal plate structure via solid-state oxidation. Our results indicate that Si has the potential to cause GR to form in smaller particles and upon air oxidation, Si can either stabilize the plate structure or alter transformation to ferrihydrite.

36 MATERIALS SCIENCE↗
DOE OSTI2024

ZeroCAL: Eliminating Carbon Dioxide Emissions from Limestone’s Decomposition to Decarbonize Cement Production

Limestone (calcite, CaCO 3 ) is an abundant and cost-effective source of calcium oxide (CaO) for cement and lime production. However, the thermochemical decomposition of limestone (~800 °C, 1 bar) to produce lime (CaO) results in substantial carbon dioxide (CO 2(g) ) emissions and energy use, i.e., ~1 tonne [t] of CO 2 and ~1.4 MWh per t of CaO produced. Here, we describe a new pathway to use CaCO 3 as a Ca source to make hydrated lime (portlandite, Ca(OH) 2 ) at ambient conditions (p, T) while nearly eliminating process CO 2(g) emissions (as low as 1.5 mol. % of the CO 2 in the precursor CaCO 3 , equivalent to 9 kg of CO 2(g) per t of Ca(OH) 2 ) within an aqueous flowelectrolysis/ pH-swing process that coproduces hydrogen (H 2(g) ) and oxygen (O 2(g) ). Because Ca(OH) 2 is a zero-carbon precursor for cement and lime production, this approach represents a significant advancement in the production of zero-carbon cement. The Zero CArbon Lime (ZeroCAL) process includes dissolution, separation/recovery, and electrolysis stages according to the following steps: (Step 1) chelator (e.g., ethylenediaminetetraacetic acid, EDTA)-promoted dissolution of CaCO 3 and complexation of Ca 2+ under basic (>pH 9) conditions, (Step 2a) Ca enrichment and separation using nanofiltration (NF), which allows separation of the Ca-EDTA complex from the accompanying bicarbonate (HCO 3 – ) species, (Step 2b) acidity-promoted decomplexation of Ca from EDTA, which allows near-complete chelator recovery and the formation of a Ca-enriched stream, and (Step 3) rapid precipitation of Ca(OH) 2 from the Ca-enriched stream using electrolytically produced alkalinity. These reactions can be conducted in a seawater matrix yielding coproducts including hydrochloric acid (HCl) and sodium bicarbonate (NaHCO 3 ), resulting from electrolysis and limestone dissolution, respectively. Careful analysis of the reaction stoichiometries and energy balances indicates that approximately 1.35 t of CaCO 3 , 1.09 t of water, 0.79 t of sodium chloride (NaCl), and ~2 MWh of electrical energy are required to produce 1 t of Ca(OH) 2 , with significant opportunity for process intensification. This approach has major implications for decarbonizing cement production within a paradigm that emphasizes the use of existing cement plants and electrification of industrial operations, while also creating approaches for alkalinity production that enable cost-effective and scalable CO 2 mineralization via Ca(OH) 2 carbonation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Computer simulation of reaction and transport of core-scale serpentinization of Fe-bearing olivine and evolution of geological hydrogen

We present reactive flow and transport simulations of core-scale serpentinization of forsteritic, Fe-bearing olivine under hydrothermal conditions. The model captures fluid flow, evolving porosity–permeability, and redox-controlled H 2 production in a cylindrical core over 55 days at 245 °C and 37 bar. Key processes include olivine dissolution, precipitation of serpentine and magnetite, and oxidation of Fe2+ to Fe 3+ . Here, results show strong coupling among flow velocity, alteration front propagation, and spatially heterogeneous H 2 generation. Elevated H2 concentrations align with inlet-localized magnetite precipitation, consistent with experiments. Secondary mineral formation reduces porosity and permeability, altering transport pathways. Reactive flow at the fluid–solid interface governs H 2 generation rates and distribution. Dissolved SiO2 promotes serpentine and talc formation by suppressing brucite, while bicarbonate extends reaction duration and moderates surface complexation effects.

Geologic hydrogen↗
NASA NTRS1998

The role of biomineralization in microbiologically influenced corrosion

Synthetic iron oxides (goethite, alpha-FeO.OH; hematite, Fe2O3; and ferrihydrite, Fe(OH)3) were used as model compounds to simulate the mineralogy of surface films on carbon steel. Dissolution of these oxides exposed to pure cultures of the metal-reducing bacterium, Shewanella putrefaciens, was followed by direct atomic absorption spectroscopy measurement of ferrous iron coupled with microscopic analyses using confocal laser scanning and environmental scanning electron microscopies. During an 8-day exposure the organism colonized mineral surfaces and reduced solid ferric oxides to soluble ferrous ions. Elemental composition, as monitored by energy dispersive x-ray spectroscopy, indicated mineral replacement reactions with both ferrihydrite and goethite as iron reduction occurred. When carbon steel electrodes were exposed to S. putrefaciens, microbiologically influenced corrosion was demonstrated electrochemically and microscopically.

Non-programmatic↗
DOE OSTI2024

Effect of glass forming additives on low-activity waste feed conversion to glass

A significant effort was invested in the past to develop and refine mathematical models that relate the composition of nuclear waste glasses with their properties, such as viscosity, electrical conductivity, or chemical durability. However, less attention has been paid to the formulation of the melter feed itself, such as the chemical form and the particle size of the glass forming and modifying additives (GFMA), which have a significant effect on the feed-to-glass conversion process during melting. To address this issue, we systematically changed the mineral composition of a simulated low-activity waste melter feed and inspected its melting behavior. When substituting minerals with corresponding oxides and hydroxides, we found that different alumina sources (kyanite, gibbsite, boehmite, or corundum) had the strongest effect on the feed melting process, whereas the sources of Ca, Mg, and Zr had little effect. Further, the x-ray diffraction analysis showed that the alumina sources differ in their dissolution kinetics: early dissolving alumina sources, such as gibbsite (Al(OH) 3 ) and boehmite (AlO(OH)), increase the transient glass-forming melt viscosity at early stages, when gases still evolve, causing extended foaming, whereas alumina sources that dissolve at high temperatures, such as kyanite (Al 2 SiO 5 ) and corundum (Al 2 O 3 ), keep the transient glass-forming melt viscosity low and lead to a faster foam collapse. Using viscosity-composition relationship to estimate the viscosity of transient glass-forming melts in the primary foaming range, we found that the primary foam began to collapse at 360 to 800 Pa s, and fully collapsed between 65 and 260 Pa s. This result agrees with our previous studies, according to which the glass-forming melt viscosity at the cold cap foam bottom ranged from 24 to 85 Pa s.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗