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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A general mechanism for gel layer formation on borosilicate glass under aqueous corrosion

Mineral and glass dissolution is a scientific topic deeply investigated but incompletely understood and of a great interest for the geochemical and materials science communities. If the interfacial dissolution/reprecipitation mechanism seems to be applicable to most of silicate minerals, the debate remains open concerning glass. Here we studied two model glasses, a ternary borosilicate (CJ1) and the same glass doped with 4.1 mol% of Al2O3 (CJ2). The two glasses were altered at 90°C, pH 9, and in conditions far and close to saturation with respect to amorphous silica, to determine the initial and residual rates. Moreover, a specific experiment was conducted for a short duration with a solution highly enriched with 18O and 29Si isotopes to understand how passivating gels form. SEM, TEM and ToF-SIMS characterization, along with Monte Carlo simulations were used to understand the rate limiting reactions at play and infer the role of Al. We show that Al yields a slower matrix dissolution in dilute conditions. However, it slows down he formation and the maturation of the passivating gel and favors alteration by partial hydrolysis of Si and Al entities followed by in-situ reorganization/relaxation into a porous network. Unexpectedly, CJ1 experienced both interfacial dissolution/reprecipitation and partial hydrolysis followed by in situ reorganization of the silicate network during the course of a single experiment. This study offers a unified concept that can pave the way for the future development of a predictive kinetic model based on a detailed description of bond breaking and bond forming as a function of glass composition and alteration conditions.

Gin, Stephane↗
DOE OSTI2020

Reactive chemical transport simulations of geologic carbon sequestration: Methods and applications

Chemical reaction simulations are considerably used to quantitatively assess the long-term geologic carbon sequestration (GCS), such as CO 2 sequestration capacity estimations, leakage pathway analyses, enhanced oil recovery (EOR) efficiency studies, and risk assessments of sealing formations (caprocks), wellbores, and overlying underground water resources. All these require a deep understanding of the CO 2 - associated chemical reactions. To ensure long-term, safe CO 2 sequestration in the intended formations, modeling is the only way to plausibly assess the CO 2 flow, reaction, and transport over thousands of years. This review summarizes the multiple methodologies for describing homogeneous and heterogeneous chemical reaction patterns and multiscale application examples, the recent progress and current status of chemical reaction simulations for GCS, and the impact of such simulations on geological CO2 sequestration performance. Technical gaps and future challenges are also discussed for further study. The trends and challenges of such studies include: (1) the combination of coupled chemical, mechanical, and transport processes with calibrated experiments and associated uncertainty/risk assessments; (2) enhancement of the ability to simulate detailed geophysical and geochemical equations to mimic in situ conditions; and (3) characterization of multiscale subsurface systems with detailed conceptual models and assignment of suitable boundary conditions for field-scale sequestration fields. One major gap remaining is the current lack of accurate (and scale-justified) kinetic and equilibrium chemical reaction parameters under reservoir conditions. Advanced models that couple chemical, mechanical, and transport processes with scale-justified parameters, from lab to field-scale experiments, are required for quantitative assessments of sequestration capacity and the long-term safety of GCS projects.

58 GEOSCIENCES↗
NASA NTRSDate not supplied

Testing and Application of Commercial Thermodynamics Software for Solid-Gas Equilibria in Planetary Science Applications

The ability to calculate chemical equilibria from thermochemical constants (e.g., H, S, Cp) or other experimental data is a tool widely employed by scientists. However, phase equilibria for planetary science problems is limited by easy access to libraries of thermochemical data, as well as the software to invert that data. Many academic software packages are focused on specific types of problems (e.g., aqueous solutions or melting and crystallization of magmas). This focus makes them excellent tools for specific uses, but poorer tools for other scenarios, especially those involving elements or chemical species that are less well-studied in that specific scientific field (e.g. NaCl vapor). Amongst the more general thermodynamic software tools, there are closed academic software packages, open-source options, as well as commercial software. We have explored the extent to which commercial chemistry/chemical engineering software may be able to satisfy the need for thermochemical modeling packages that can accommodate the diverse species and conditions of planetary science problems. Here we compare the output of software package HSC Chemistry™ (Metso Outotec) to published vapor-solid phase diagrams for a variety of major and minor elements. HSC Chemistry™ has been used in several recent geochemical studies of terrestrial volcanic systems [2- 4]. However, it has not to our knowledge been benchmarked against peer-reviewed model results for the conditions and compositions relevant to planetary science. We present one such comparison here, the low- pressure environment of the solar nebula, using literature data. In short, we find excellent agreement between HSC Chemistry™ and the well-regarded academic software package CONDOR. These preliminary results suggest that at least some commercial software packages are capable of robust thermochemical calculations for planetary science.

planetary science↗
DOE OSTI2024

​Understanding a Stratigraphic Hydrothermal Resource – Geophysical Imaging at Steptoe Valley, Nevada

Sandia National Laboratories partnered with a multi-disciplinary group of subject matter experts to evaluate a stratigraphic geothermal resource in Steptoe Valley, Nevada using both established and novel geophysical imaging techniques. The stratigraphic reservoir in northern Steptoe Valley was previously discovered during oil and gas exploration. Subsequent studies, such as the Nevada Play Fairway Analysis, included data which further highlighted potential resource targets in the basin. Geophysical surveys, complemented with refined geologic mapping and geochemical sampling, were deployed to further characterize the resource. The resulting 3D geologic interpretation, conceptual model refinements, and reservoir simulations suggest that a >100MWe power-capable reservoir is likely economically accessible using conventional well placement and stimulation techniques in the Paleozoic carbonates of the deep/central basin of northern Steptoe Valley. Additional geophysical characterization and exploration drilling efforts are recommended to calibrate interpretation and determine where/how to potentially develop the northern Steptoe resource. The geophysical tools, interpretations, lessons learned, and public data generated by this study establish an exploration methodology to inform decisions for characterization and development of northern Steptoe Valley and other stratigraphic geothermal reservoirs in the western U.S.

15 GEOTHERMAL ENERGY↗
NASA NTRS1985

Basalts of Mars: Constraints on Volatile Evolution

The mineralogy of relatively unweathered rocks on Mars place important constraints on models of planetary oxidation state, volcanism and associated outgassing, accretion and associated volatile inventory, and geochemical changes over time. Reflectance spectra (300 to 2500 nm) provide direct mineralogic information about the surface materials. Spectra measured using Earth-based telescopes were analyzed by a multiple high-order derivative spectroscopy technique. Nine areas, measured during the 1978 opposition, were analyzed by the technique. Each contained suites of well-defined absorption bands. These bands can be interpreted in terms of constituent mineralogy by the technique of Adams. Among the features extracted from the spectra were bands attributed to iron oxides. Other bands can be attributed to silicates within chemically unweathered rocks/fines. Absorption features suggest the presence of Mg-olivine and plagioclase feldspar.

Huguenin, R. L.↗
NASA NTRS1991

Spectroscopy and reactivity of mineral analogs of the Martian soil

To answer the question of why life occurred on Earth but not on Mars requires a study of the geochemical and physical aspects of the Martian soil. Some of the best Mars analog mineral models of the soil have been prepared and justified according to known constraints of chemical composition, reflectance spectroscopy, and chemical reactivity. Detailed laboratory reflectance spectra in the ultraviolet, visible, and near infrared (.30 to 2.5 microns) and the infrared (2.5 to 25 microns) regions have been obtained for the pure candidate minerals and some analog mixtures and compared to Mars reflectance spectra. Modeling of the reflectance spectra from optical constraints determined for the analog minerals has begun and will be interpreted in terms of the effects of particle size variation, component mixing, and soil packing upon remotely sensed reflectance spectra. This has implications not only for Mars, but for other planets and planetoids. The ratio of Fe(II)/Fe(III) in the Martian soil analog materials on spectral reflectance in the visible range has begun, and the results will be evaluated according to conformity with the visible Mars reflectance spectrum. Some initial LR and GEX data have been collected for the mineral samples and their mixtures, which can be compared with the Viking data and interpreted in terms of the redox (Fe(II)/Fe(III) environment.

Banin, A.↗
NASA NTRS2000

Scientific Objectives of the Mars Surveyor 2001 Gamma-Ray Spectrometer

The Gamma-Ray Spectrometer (GRS) is one of the instruments on the Mars Surveyor 2001 Orbiter, which is part of NASA's Mars-Surveyor program. The GRS is really an instrument suite consisting of the GRS, a neutron spectrometer (NS), and a high-energy neutron detector (FIEND). Each of these instruments/sensors are remotely mounted at different locations on the spacecraft and connect to a central electronics box. The GRS will achieve global mapping of the elemental composition of the surface and the abundance of hydrogen in the shallow subsurface. It is an updated design using the same technology as the lost Mars Observer mission. The Martian surface is continuously bombarded by cosmic ray particles; their interactions with the constituents of the soil produces nuclear reaction cascades with fast neutrons being the main secondaries. Those neutrons interact in turn with the nuclei of the elements that make up the soil and they eventually get slowed to thermal energies. In this process they leave the nuclei in an excited state that decays via the emission of characteristic gamma rays. All these processes are precisely known and have been simulated by means of numerical models. Thus, remote gamma-ray spectroscopy is a useful method for quantitatively measuring the geochemical composition of the surface down to a few tens of g/sq cm. Additional information is contained in original extended abstract.

Boynton, W. V.↗
NASA NTRS1988

Thematic mapper study of Alaskan ophiolites

The two principle objectives of the project Thematic Mapper Study of Alaskan Ophiolites were to further develop techniques for producing geologic maps, and to study the tectonics of the ophiolite terrains of the Brooks Range and Ruby Geanticline of northern Alaska. Ophiolites, sections of oceanic lithosphere emplaced along island arcs and continental margins, are important to the understanding of mountain belt evolution. Ophiolites also provide an opportunity to study the structural, lithologic, and geochemical characteristics of ocean lithosphere, yielding a better understanding of the processes forming lithosphere. The first part of the report is a description of the methods and results of the TM mapping and gravity modeling. The second part includes papers being prepared for publication. These papers are the following: (1) an analysis of basalt spectral variations; (2) a study of basalt geochemical variations; (3) an examination of the cooling history of the ophiolites using radiometric data; (4) an analysis of shortening produced by thrusting during the Brooks Range orogeny; and (5) a study of an ophiolite using digital aeromagnetic and topographic data. Additional papers are in preparation.

Bird, John M.↗
DOE OSTI2022

BioRT-Flux-PIHM v1.0: a biogeochemical reactive transport model at the watershed scale

Watersheds are the fundamental Earth surface functioning units that connect the land to aquatic systems. Many watershed-scale models represent hydrological processes but not biogeochemical reactive transport processes. This has limited our capability to understand and predict solute export, water chemistry and quality, and Earth system response to changing climate and anthropogenic conditions. Here we present a recently developed BioRT-Flux-PIHM (BioRT hereafter) v1.0, a watershed-scale biogeochemical reactive transport model. The model augments the previously developed RT-Flux-PIHM that integrates land-surface interactions, surface hydrology, and abiotic geochemical reactions. It enables the simulation of (1) shallow and deep-water partitioning to represent surface runoff, shallow soil water, and deeper groundwater and of (2) biotic processes including plant uptake, soil respiration, and nutrient transformation. The reactive transport part of the code has been verified against the widely used reactive transport code CrunchTope. BioRT-Flux-PIHM v1.0 has recently been applied in multiple watersheds under diverse climate, vegetation, and geological conditions. This paper briefly introduces the governing equations and model structure with a focus on new aspects of the model. It also showcases one hydrology example that simulates shallow and deep-water interactions and two biogeochemical examples relevant to nitrate and dissolved organic carbon (DOC). These examples are illustrated in two simulation modes of complexity. One is the spatially lumped mode (i.e., two land cells connected by one river segment) that focuses on processes and average behavior of a watershed. Another is the spatially distributed mode (i.e., hundreds of cells) that includes details of topography, land cover, and soil properties. Whereas the spatially lumped mode represents averaged properties and processes and temporal variations, the spatially distributed mode can be used to understand the impacts of spatial structure and identify hot spots of biogeochemical reactions. The model can be used to mechanistically understand coupled hydrological and biogeochemical processes under gradients of climate, vegetation, geology, and land use conditions.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1985

Biological modulation of planetary atmospheres: The early Earth scenario

The establishment and subsequent evolution of life on Earth had a profound impact on the chemical regime at the planet's surface and its atmosphere. A thermodynamic gradient was imposed on near-surface environments that served as the driving force for a number on important geochemical transformations. An example is the redox imbalance between the modern atmosphere and the material of the Earth's crust. Current photochemical models predict extremely low partial pressures of oxygen in the Earth's prebiological atmosphere. There is widespread consensus that any large-scale oxygenation of the primitive atmosphere was contingent on the advent of biological (autotrophic) carbon fixation. It is suggested that photoautotrophy existed both as a biochemical process and as a geochemical agent since at least 3.8 Ga ago. Combining the stoichiometry of the photosynthesis reaction with a carbon isotope mass balance and current concepts for the evolution of the stationary sedimentary mass as a funion of time, it is possible to quantify, the accumulation of oxygen and its photosynthetic oxidation equivalents through Earth history.

Schidlowski, M.↗
NASA NTRS2017

Investigating Weathering of Basaltic Materials in Gale Crater, Mars: A Combined Laboratory, Modeling and Terrestrial Field Approach

Recent observations from Gale Crater, Mars document past aqueous alteration both in the formation of the Stimson sandstone unit, as well as in the formation of altered fractures within that unit. Geochemical and mineralogical data from Curiosity also suggest Fe-rich amorphous weathering products are present in most samples measured to date. Here we interpret conditions of possible past weathering in Gale Crater using a combination of field, laboratory, and modeling work. In order to better understand secondary Fe-rich phases on Mars, we are examining formation of weathering products in high Fe and Mg and low Al serpentine soils in the Klamath Mountains, CA. We have isolated potential weathering products from these soils, and are analyzing them using synchrotron μXRF and μXRD as well as FullPat for a direct comparison to analyses from Gale Crater. In order to interpret the implications of the persistence of potential secondary Fe-containing phases on Mars, we are also measuring the dissolution rates of the secondary weathering products allophane, Fe-rich allophane, and hisingerite. Ongoing dissolution experiments of these materials suggest that they dissolve significantly more rapidly than more crystalline secondary minerals with similar chemical compositions. Finally, to quantify the specific conditions of past aqueous alteration in Gale Crater we are performing reactive transport modeling of a range of possible past environmental conditions. Specifically, we are testing the conditions under which a Stimson unit-like material forms from a parent material similar to Rocknest or Bagnold eolian deposits, and the conditions under which observed altered fracture zones form from a Stimson unit-like parent material. Our modeling results indicate that the formation of the Stimson unit is consistent with leaching of an eolian deposit with a solution of pH = 6-8, and that formation of the altered fracture zones is consistent with leaching with a very acidic (pH = 2-3) high sulfate solution containing Ca. These results suggest circumneutral pH conditions during authigenesis or early diagenesis in the Stimson formation sediments followed by diagenetic alteration by very acidic solutions along fracture zones.

Hausrath, Elisabeth↗
DOE OSTI2020

A Perspective on the Successes of the NNSS Underground Test Area (UGTA) Activity - 20221

Between 1951 and 1992, 828 underground nuclear tests were performed at the Nevada National Security Site (NNSS). Underground testing was done in five major testing areas, which included (1) Frenchman Flat, (2) Rainier Mesa/Shoshone Mountain, (3) Yucca Flat/Climax Mine (4) Central Pahute Mesa, and (5) Western Pahute Mesa. About one third of the underground tests were detonated near, at or below the water table, and thus radioactive contamination was introduced to the groundwater system. The U.S. Department of Energy's Underground Test Area (UGTA) Activity was established in the late 1990's to address the fate and movement of residual radioactivity in groundwater, and characterize the risk that it may pose to NNSS workers and the offsite public. It has accomplished this goal through a process of iterative groundwater sampling and numerical groundwater flow and transport modeling, and long-term monitoring. The UGTA Activity draws on the expertise of scientists in the fields of geology, hydrology, radiochemistry, and risk assessment from the U.S. DOE staff, the lead contractor (currently Navarro) and many other organizations, in cooperation with the governing regulatory body, the State of Nevada's Division of Environmental Protection (NDEP). Los Alamos National Laboratory (LANL) is one of the participating research organizations involved with the UGTA Activity. Under the direction of DOE and the lead contractor, LANL's role in UGTA has evolved over time from an initial focus on geologic characterization, to conducting field and laboratory experiments, and finally to its current role of providing modeling and geochemistry expertise to characterize the rates and directions of groundwater and radionuclide movement. In its current role, LANL has either developed or provided the numerical tools for developing flow and transport models in each of the four major testing areas. In addition, LANL has provided an independent assessment of future groundwater flow and transport behavior through the analysis of naturally-occurring geochemical and isotopic tracers in groundwater. The five major testing areas are now in different stages of investigation or closure: (1) Frenchman Flat is in its fifth year of post closure modeling; (2) The Rainier Mesa/Shoshone Mountain Closure Report has been submitted to NDEP and is awaiting approval; (3) The Yucca Flat/Climax Mine Closure Report is under development; and (4) Central and (5) Western Pahute Mesa is still undergoing investigation and flow and transport model development. The success of the UGTA Activity in reaching or approaching closure in three of the five major testing areas is primarily due to the DoE's focus on regulatory closure requirements, but also is in part attributable to a rigorous internal review process and the involvement of NDEP and Nye County water professionals as participants and observers in the reviews. County and state involvement in the internal review process has promoted trust that the U.S. DOE is deeply committed to ensuring the present and future safely of NNSS workers and the surrounding communities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS2018

Reactive Transport and Mass Balance Modeling of the Stimson Sedimentary Formation and Altered Fracture Zones Constrain Diagenetic Conditions at Gale Crater, Mars

On a planet as cold and dry as present-day Mars, evidence of multiple aqueous episodes offers an intriguing view into very different past environments. Fluvial, lacustrine, and eolian depositional environments are being investigated by the Mars Science Laboratory Curiosityin Gale crater, Mars. Geochemical and mineralogical observations of these sedimentary rocks suggest diagenetic processes affected the sediments. Here, we analyze diagenesis of the Stimson formation eolian parent material, which caused loss of olivine and formation of magnetite. Additional, later alteration in fracture zones resulted in preferential dissolution of pyroxene and precipitation of secondary amorphous silica and Ca sulfate. The ability to compare the unaltered parent material with the reacted material allows constraints to be placed on the characteristics of the altering solutions. In this work we use a combination of a mass balance approach calculating the fraction of a mobile element lost or gained, τ, with fundamental geochemical kinetics and thermodynamics in the reactive transport code CrunchFlow to examine the characteristics of multiple stages of aqueous alteration at Gale crater, Mars. Our model results indicate that early diagenesis of the Stimson sedimentary formation is consistent with leaching of an eolian deposit by a near-neutral solution, and that formation of the altered fracture zones is consistent with a very acidic, high sulfate solution containing Ca, P and Si. These results indicate a range of past aqueous conditions occurring at Gale crater, Mars, with important implications for past Martian climate and environments.

Gale crater↗
NASA NTRS1991

Biogeochemical modeling at mass extinction boundaries

The causes of major mass extinctions is a subject of considerable interest to those concerned with the history and evolution of life on earth. The primary objectives of the proposed plan of research are: (1) to develop quantitative time-dependent biogeochemical cycle models, coupled with an ocean atmosphere in order to improve the understanding of global scale physical, chemical, and biological processes that control the distribution of elements important for life at times of mass extinctions; and (2) to develop a comprehensive data base of the best available geochemical, isotopic, and other relevant geologic data from sections across mass extinction boundaries. These data will be used to constrain and test the biogeochemical model. These modeling experiments should prove useful in: (1) determining the possible cause(s) of the environmental changes seen at bio-event boundaries; (2) identifying and quantifying little-known feedbacks among the oceans, atmosphere, and biosphere; and (3) providing additional insights into the possible responses of the earth system to perturbations of various timescales. One of the best known mass extinction events marks the Cretaceous/Tertiary (K/T) boundary (66 Myr ago). Data from the K/T boundary are used here to constrain a newly developed time-dependent biogeochemical cycle model that is designed to study transient behavior of the earth system. Model results predict significant fluctuations in ocean alkalinity, atmospheric CO2, and global temperatures caused by extinction of calcareous plankton and reduction in the sedimentation rates of pelagic carbonates and organic carbon. Oxygen-isotome and other paleoclimatic data from K/T time provide some evidence that such climatic fluctuations may have occurred, but stabilizing feedbacks may have acted to reduce the ocean alkalinity and carbon dioxide fluctuations.

Rampino, M. R.↗
NASA NTRS2018

Reactive Transport and Mass Balance Modeling of the Stimson Sedimentary Formation and Altered Fracture Zones Constrain Diagenetic Conditions at Gale Crater, Mars

On a planet as cold and dry as present-day Mars, evidence of multiple aqueous episodes offers an intriguing view into very different past environments. Fluvial, lacustrine, and eolian depositional environments are being investigated by the Mars Science Laboratory Curiosity in Gale crater, Mars. Geochemical and mineralogical observations of these sedimentary rocks suggest diagenetic processes affected the sediments. Here, we analyze diagenesis of the Stimson formation eolian parent material, which caused loss of olivine and formation of magnetite. Additional, later alteration in fracture zones resulted in preferential dissolution of pyroxene and precipitation of secondary amorphous silica and Ca sulfate. The ability to compare the unaltered parent material with the reacted material allows constraints to be placed on the characteristics of the altering solutions. In this work we use a combination of a mass balance approach calculating the fraction of a mobile element lost or gained, tau, with fundamental geochemical kinetics and thermodynamics in the reactive transport code CrunchFlow to examine the characteristics of multiple stages of aqueous alteration at Gale crater, Mars. Our model results indicate that early diagenesis of the Stimson sedimentary formation is consistent with leaching of an eolian deposit by a near-neutral solution, and that formation of the altered fracture zones is consistent with a very acidic, high sulfate solution containing Ca, P and Si. These results indicate a range of past aqueous conditions occurring at Gale crater, Mars, with important implications for past martian climate and environments.

Gale↗
NASA NTRSDate not supplied

Modeling the Crystallization of Martian Igneous Compositions

The martian crust is dominated by basalts and ultramafic rocks [1]. Understanding the crystallization sequence of martian igneous rocks is critical for constraining the petrologic and geochemical evolution of the crust and mantle. Experimental studies have investigated the parental liquid compositions and crystallization behavior using martian meteorite compositions [2-7], as well as compositions measured by rovers on the martian surface [8,9]. While experiments deliver crucial results, they are often limited by time and resources. Therefore, modeling approaches are an ideal tool to complement experimental results. The application of the MELTS software package [10, 11], to calculate the crystallization of martian compositions, reproduces important compositional details of magma crystallization but significant uncertainties regarding the pressure of the olivine-pyroxene multiple saturation point have been reported [12], and in the temperatures of initial crystallization [12, 13]. Recently, a new melting model, MAGMARS, has been shown to reproduce martian primary melts more accurately [14]. Here, we constrain the applicability of Gibbs free energy minimization software Perple_X [15] for martian compositions by comparing our modeled results to experimentally derived crystallization paths for two martian compositions.

J Semprich↗
DOE OSTI2020

Engineered Barrier System R&D and International Collaborations – LANL (FY20): Spent Fuel and Waste Disposition

The United States Department of Energy’s Spent Fuel and Waste Disposition (SFWD) program is investigating the design and safety function of generic nuclear geologic repositories in a variety of geologic settings (salt, argillite, and crystalline rock). Different configurations and loadings of spent nuclear fuel and waste within disposal canisters are also being investigated, some of which have the potential to generate repository temperatures higher than previously considered (i.e., temperatures >100ºC) by foreign and domestic concepts. This report expands on engineered barrier material stability in a high temperature crystalline rock repository through high temperature hydrothermal experiments. Experiments were designed to develop engineered barrier system (EBS) concepts in a hightemperature crystalline environment in 1) bentonite-Grimsel Granodiorite interactions, 2) bentonite-cement reactions, and 3) interaction between waste canister materials and bentonite. Experiment results are applied to understanding long-term repository performance in terms of radionuclide isolation. One hydrothermal experiment was completed in the rocking autoclaves at LANL in FY-20: IEBS-6 (Grimsel Granodiorite + Wyoming bentonite + cured ordinary Portland cement + Grimsel Granodiorite synthetic groundwater, 250ºC/150 bar, 8 weeks). Several other experiments were planned but were delayed due to the COVID-19 pause in laboratory work. In addition, some characterization of the reaction products of experiments conducted in FY-20 was prevented by COVID-19. Mineral phase chemistry was not measured via electron microprobe analyses for IEBS-6. Quantitative X-ray diffraction results from IEBS-6 and HBT-1 were not completed. The missing analyses and discussion of the results will be included in next year’s report. New characterization that was completed includes scanning electron microscopy of reaction products from IEBS-6, quantitative X-ray diffraction results are presented from IEBS-1 through IBES-5, preliminary scanning electron microscope images and chemical analyses for IEBS-6, X-ray diffraction of the clay fraction from all experiments, measurement/imaging of mineral growth on the surface of steel coupons. Major observations pertaining to bentonite stability in a Grimsel Granodiorite environment include the stability of Na-montmorillonite at 250°C, the formation of trace CSH phases, and the formation of bentonite colloids on experiment cooling. The addition of a cured chip of Portland cement to the bentonite-Grimsel system results in slightly higher pH values and the formation of diverse secondary mineral phases that were not observed in the previous experiments (e.g., analcime, garronite, CSH phases). The new characterization efforts related to the interaction of stainless-steel coupons and bentonite clay focused on thickness and mineralogy of phases that formed at the steel surface. In Wyoming bentonite + Grimsel Granodiorite systems, newly formed minerals at the bentonitesteel coupon interface included alteration of the outermost steel edge to Fe,Cr-oxide phases, followed by Fe-rich phyllosilicates (Fe-saponite, chlorite) and interbedded Fe,Cr,Ni-sulfide phases (pentlandite). Hydrothermal experiments were completed to assess uranium-carbonate complexation at conditions relevant to high-temperature disposal. Autoclave solubility experiments were conducted at 150 to 250ºC with a range of carbonate and uranium concentrations. The experiment results were characterized via situ UV-Visible spectroscopy and synchrotron-based in situ XAS techniques. Results show a significant decrease in the stability of uranyl-carbonate complexes at temperatures above 100ºC along with the precipitation of uranium oxides. Further, at T > 200ºC, results show that uranyl-hydroxyl complexes control solubility of uranium instead of the previously predicted uranyl-carbonate species. These results are significant for understanding the mobility of uranium in the EBS, which will likely contain carbonate-rich fluids. International research efforts focused on three main areas: 1) participation in international conferences, 2) building collaborations with foreign repository programs, and 3) the initiation of an experimental program to complement the full-scale HotBENT test at the Grimsel test site. This experiment included Wyoming bentonite + low carbon steel + Grimsel Granodiorite synthetic groundwater and was run at the planned maximum temperature of the HotBENT test (200°C). Complete characterization of reaction products was hindered by disruptions to laboratory work but will be reported in the next FY. The experimental results obtained in FY-20 continue to document the wide-ranging effects of bulk composition and pressure-temperature conditions in the mineralogical and geochemical evolution of a high-temperature repository environment. Concepts developed will be used to inform models of long-term material stability in a generic crystalline rock-hosted repository.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1988

An illustration of the complexity of continent formation

It was pointed out that a consensus may be emerging in crustal growth models, considering the clustering of most growth curves and their uncertainties. Curves most distant from this clustering represent models involving extensive recycling of continental material back into the mantle, but the author wondered if geochemical signatures for this would be recognizable considering the lack of evidence from seismic tomography for discrete mantle reservoirs, and the likelihood of core-mantle interaction based on recent high pressure experiments. Unreactivated Archean rocks represent only 2 percent of present continental area, and the author was uncomfortable about basing inferences on what the early Earth was like on such a small amount of information. He feels that the hypothesis of continental assembly that needs testing is that of banging together of island arcs, such as in Indonesia today. As an example of how complex this process can be, the author described the geology of the Caribbean arc system, which shows evidence for reversals of subduction polarity, numerous collisional events, and substantial strike-slip movements. It seemed unlikely to the author that Archean examples would have been less complicated.

Burke, Kevin↗