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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Graphene nanoplatelets reinforced cement as a solution to leaky wellbores reinforcing weak points in hydrated Portland cement with graphene nanoparticles improves mechanical and chemical durability of wellbore cements

In this work, to improve the performance of wellbore cement under subsurface environments, graphene nanoplatelets (GNPs) were added in various percentages to Class-H cement slurry. Microstructural characterization of cement slurries cured at 90 °C and 95% RH indicates that GNP modifies the microstructure of hydrated cement by reinforcing pore spaces. As a result, the mechanical properties, such as Young's modulus and axial peak stress, obtained from high temperature triaxial compression tests are significantly improved based on different percentages of added GNPs. Furthermore, the hydrated 1 × 2 inch GNP- Portland cement cores tested under simulated deep wellbore conditions of high-temperature and high pressure (HTHP), appear to have a ductile-like behavior, when compared to a typical brittle nature of Portland cement pastes. From our observations and published data on graphene resistance to fracture, GNP addition to cement is evidently enhancing the flexibility of cement. These improvements would reduce the risks associated with wellbore cement deterioration and a consequent leakage in fossil fuel production, geothermal energy production, CO 2 storage as well as long-term sealing materials in plugging and abandonment of all wellbores at the end of their service life.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Insights into the physical and chemical properties of a cement-polymer composite developed for geothermal wellbore applications

To isolate injection and production zones from overlying formations and aquifers during geothermal operations, cement is placed in the annulus between well casing and formations. Wellbore cement can fracture due to chemical and physical stress. A polymer-cement (composite) with self-healing properties, stable at high temperatures, was recently developed by our group. Here we present data on the elemental distribution, mineral composition, internal microstructure, and tensile elasticity of this composite and how it compares to cement without polymer (control cement). Entrapped air porosity was similar between control cement (0.44% by volume) and composite (0.22% by volume). Total voids increased with polymer content in the cement (10% and 25% composite), and polymer was found to fill most of these voids. Polymer appears to act as a (cement hydration) retarder increasing the amount of unhydrated silicate minerals in the matrix. Tensile elasticity was improved for composites as compared to control cement, suggesting that the composite materials perform better under mechanical stress. Density-functional calculations reproduce the drop in Young’s modulus by about 60% observed experimentally when polymer is added to the cement. In addition, calculations indicate that the bonding interactions between the cement and polymer remain stable over the range of strain studied.

Rod, Kenton A. (ORCID:0000000318189094)↗
DOE OSTI2021

Structural and chemical changes from CO2 exposure to self-healing polymer cement composites for geothermal wellbores

Wellbore cement is subjected to a number of mechanical, thermal and chemical stress regimes over its lifetime. Therefore, next generation wellbore cement formulations need to be evaluated in conditions relevant to these environments. In this work, we investigate the mechanism of the alteration of a novel self-healing polymer-cement composite recently reported by our group after exposure to a CO2-rich environment by using synchrotron based X-ray Fluorescence (XRF) and X-ray absorption near edge structure (XANES) and scanning electron microscopy coupled with energy dispersive spectroscopy. Results showed that chemical alteration of the polymer-cement follows the rim carbonation mechanism, similar to conventional cement although carbonation takes place to a lesser extent in polymer-cements despite the higher porosity. Along with detailed mechanistic insights on carbonation in polymer-cement composite, the performance of these in CO2-rich environment is further studied using standard compressive strength analysis.

Elbakhshwan, Mohamed↗
DOE OSTI2021

Cement stress and microstructure evolution during curing in semi-rigid high-pressure environments

The process of cement slurry curing into a solid has a direct effect on the initial state of stress in a composite concrete and steel structure. Failure models for critical infrastructure and wellbores could benefit from measurements of this initial stress because it greatly influences structural performance. Here, we present measurements of the initial stress state (total stress, effective stress, and pore pressure) of multiple cement formulations cured under a high-pressure of 40 MPa within a semi-rigid steel pipe. Our results show that cements cured in this restrained environment exhibit dense microstructures with low permeability (nano-Darcy), develop an anisotropic stress state greater than zero and less than the curing pressure, and undergo a staged curing process where hydration and mechanical behaviors evolve from a slurry into a pre-stressed porous medium. Both drained and undrained scenarios were investigated, revealing a feedback from the semi-rigid boundary towards improved cement performance.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Enabling phase quantification of anhydrous cements via Raman imaging

The phase composition of Portland cements is typically determined using conventional techniques like X-ray Diffraction (XRD) Rietveld analysis, optical microscopy point counting, and electron microscopy. However, these techniques have several limitations that may affect their accuracy in certain sample-specific scenarios. Here, we report a highly accurate phase quantification of 11 different types of commercial, anhydrous cements using a new and complementary technique: Raman imaging. Specifically, for the 4 principal phases, composition from our extensive data (250,000 Raman spectra per sample, error < 0.71%) and those obtained from XRD Rietveld and supplier data have high coefficients of determination (R{sup 2} > 0.98, mean deviation <2%). Additionally, we also quantify 8 secondary phases present in cement clinkers (gypsum, anhydrite, bassanite, syngenite, dolomite, calcite, quartz, and portlandite) with a high degree of confidence, thereby demonstrating that Raman imaging is a highly versatile tool for anhydrous phase quantification in a broad variety of cements.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Geochemical narrowing of cement fracture aperture during multiphase flow of supercritical CO2 and brine

For carbon capture and storage operations, wells are used as a necessary conduit for injecting CO2 at depth, but they can also act as leakage conduits if the cement seals are compromised. The specific objective of this research was to investigate the nature of self-healing of a fracture within cement under multiphase flow of CO2 and brine, and to compare this to a newly developed model. This was accomplished through a laboratory investigation, flowing reacting supercritical CO2 and brine through a cement fracture with multiphase flow. The influent end of the fracture was degraded as evidenced by the formation of cracks across the surface. At the effluent end of the fracture, the initial aperture of 137 µm was reduced to 50 µm. This reduction by 87 µm was similar to results from a recently developed model tested in this study, which predicted an aperture reduction of 80 µm. Our results demonstrated that the model accurately predicted the reactions which occurred in this multiphase flow system.

wellbore, cement, fracture, multiphase-flow, super↗
DOE OSTI2021

On the use of limestone calcined clay cement (LC3) in high-strength strain-hardening cement-based composites (HS-SHCC)

Highlights: • Use of LC{sup 3} slightly reduces flowability and shortens the setting time of fresh matrices. • Highly polymerized C-A-S-H gel and abundant ettringite benefit flexural strength of LC{sup 3}-matrices. • Use of LC{sup 3} enhances the bond strength between fiber and high-strength matrix. • LC{sup 3}-based HS-SHCC yields similar flexural performance as the composite with Portland cement. High-strength strain-hardening cement-based composites (HS-SHCC) demonstrate excellent mechanical and durability properties. However, high cement content typical to HS-SHCC results not only in high carbon footprint, but also in excessive hydration heat and severe autogenous shrinkage. In this investigation, Limestone Calcined Clay Cement (LC{sup 3}) was used to produce sustainable HS-SHCC. The LC{sup 3} substitution resulted in higher energy consumption during mixing and in shorter setting times of the fresh, plain matrices. Although the LC{sup 3} substitution slightly reduced the compressive strength, the formation of highly polymerized C-A-S-H gel and abundant ettringite benefited the flexural strength of the plain matrices. Additionally, single-fiber pullout experiments showed that the use of LC{sup 3} led to increased fiber-matrix bond strength and pullout energy. Finally, the replacement of Portland cement by LC{sup 3} resulted in HS-SHCC with similar mechanical performance to the reference composite, indicating a high potential for using LC{sup 3} in high-performance cement-based composites.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Eco-efficient cements: Potential economically viable solutions for a low-CO2 cement-based materials industry

The main conclusions of an analysis of low-CO{sub 2}, eco-efficient cement-based materials, carried out by a multi-stakeholder working group initiated by the United Nations Environment Program Sustainable Building and Climate Initiative (UNEP-SBCI) are presented, based on the white papers published in this special issue. We believe that Portland-based cement approaches will dominate in the near future due to economies of scale, levels of process optimisation, availability of raw materials and market confidence. Two product-based approaches can deliver substantial additional reductions in their global CO{sub 2} emissions, reducing the need for costly investment in carbon capture and storage (CCS) over the next 20–30 years:1.Increased use of low-CO{sub 2} supplements (SCMs) as partial replacements for Portland cement clinker. 2.More efficient use of Portland cement clinker in mortars and concretes. However, other emerging technologies could also play an important role in emissions mitigation in the longer term, and thus merit further investigation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Iron speciation in blast furnace slag cements

Slag-containing pastes and concretes were analysed by element-specific synchrotron-based techniques to determine the speciation of iron on crushed materials through spatially resolved micro-spectroscopic studies. The investigated cement samples were hydrated either in the laboratory, or exposed to river or sea water. Metallic iron, along with minor proportions of iron sulphide and magnetite was detected in the laboratory sample. Iron sulphide, goethite, and siliceous hydrogarnet were discovered in the blended slag cements hydrated in contact with river water for up to 7 years. In contrast, no Fe(0) was observed in blended concretes exposed to sea water. Instead, iron sulphide, iron(II)-hydroxide and -oxide, hematite, magnetite, siliceous hydrogarnet, and goethite were detected as well as ilmenite (FeTiO{sub 3}) in the aggregates. The strong acceleration of Fe oxidation in samples exposed to sea water and the long-term passivation observed in the other samples indicate comparable processes as those occurring on steel bars.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Ettringite-Related Dimensional Stability of CO 2 -Cured Portland Cement Mortars

Carbonation curing, where cement is cured in a CO 2 -rich environment, is an emerging technology in the precast industry that promotes CO 2 sequestration in construction materials. It demonstrates good promise for enhancing material strength development, chemical resistance and manufacturing sustainability. A critically important but little studied aspect of carbonation curing is the dimensional stability of the cured materials, which poses a significant impact on longevity of cement-based materials and structures. In this study, we propose to use carbonation curing to substitute the conventional energy-intensive steam curing and time-consuming moisture curing, and examine the dimensional stability of Portland cement mortars manufactured by different curing approaches. The common pathology in precast concrete that potentially creates undesirable expansions, known as Delayed Ettringite Formation (DEF), is particularly investigated. Four curing approaches were examined including moist, steam (maximum temperature at 85°C to purposefully induce DEF), combined steam-carbonation, and carbonation curing in which steam curing was used to verify favorable cement chemistry for DEF and to indicate DEF onset timing. It was found that, among the four curing approaches designed in this study, the carbonation-cured mortars demonstrated the lowest expansion (~0%) whereas the steam-cured mortars showed the highest (>0.6%) after 500 days of storage in saturated limewater. Mortar expansion after the combined steam-carbonation curing (~0.1%) was lower than that of steam curing, but remained higher with respect to the moisture-cured reference. Here, the mineral ettringite was detected at 500 days after all curing approaches. However, larger ettringite crystal size (5-10 μm) with greater dispersion was observed via scanning electron microscopy after steam curing in reference to carbonation curing (< 5 μm). Additionally, the calcium carbonate precipitated by CO 2 carbonation was found to participate in the post-carbonation hydration to promote formation of monocarboaluminate and hemicarboaluminate, which stabilize ettringite and potentially lead to a secondary densification of the mortar microstructure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Temperature dependence of viscoelastic Poisson’s ratio of cement mortar

Abstract Concrete creep research has focused primarily on uniaxial response. However, biaxially prestressed concrete structures are common, resulting in a multiaxial stress state that can complicate the behavior of a viscoelastic material like concrete. Significant creep strains may be induced in directions transverse to each principle stress due to Poisson’s effect. Past research is unclear regarding the viscoelastic or viscoplastic properties of concrete outside of uniaxial response. It has been reported in separate studies that concrete viscoelastic/viscoplastic Poisson’s ratio (VPR) is an increasing, decreasing and constant function with time, with all reported measurements performed at room temperature. In this paper, the 3D basic creep response of mature cement mortar is examined using a confined compression experiment that allows direct determination of the full stress and infinitesimal strain tensors in a single test, which enables the determination of VPR under a multiaxial stress state. For this purpose, a unique, miniature version of the standardized concrete creep frame is designed that is amenable to placing in climate chambers and temperature ovens. The experimental results indicate that the VPR of sealed, mature cement mortar is nearly constant and equal to the elastic at room temperature, while the VPR gradually increases with time when measured at 60 °C.

Construction & Building Technology↗
DOE OSTI2021

Influence of curing temperature on belite cement hydration: A comparative study with Portland cement

Belite cements (BCs) could be a more sustainable binder than Portland cements (PCs) but adequate knowledge of the hydration features has still to be built. In particular, the mild curing hydration temperature effects have been extensively studied for PCs but not for BCs. This research was triggered by a previous work reporting improved mechanical strengths of BCs at higher curing temperatures. Here, we report the hydration characteristics of a BC at 20, 40 and 60 °C and compared to those of a typical PC. We have corroborated previous findings and used a multi-technique approach including Rietveld phase analysis, thermal analysis, calorimetry, silicon MAS-NMR, mercury intrusion porosimetry and chiefly synchrotron X-ray microtomography, to thoroughly understand the different behavior. In a nutshell, the improved mechanical performances at mild curing temperatures for BCs are mainly due to a much larger belite degree of reaction, with lower porosity coarsening of belite cements also playing a role.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Impact of cement composition, brine concentration, diffusion rate, reaction rate and boundary condition on self-sealing predictions for cement-CO 2 systems

Geological CO 2 storage (GCS) plays an important role in curbing CO 2 emissions by reducing the carbon footprint of difficult to decarbonize operations and achieve negative CO 2 emissions through activities like Bioenergy with Carbon Capture and Storage (BECCS) and Direct Air Carbon Capture and Storage (DACCS). Leakage of CO 2 through wells is an important concern when it comes to deployment of large-scale GCS. Existing wells in sites that are otherwise suitable for GCS can act as conduits for stored CO 2 to escape the reservoir. There is broad consensus that the main risk of leakage through wellbores is via fractures/damaged pathways. The results from several studies evaluating the permeability evolution of cement fractures in wells upon leakage of CO 2 agree that smaller fracture apertures, slower brine velocities and higher brine residence times promote self-sealing of fractures by mineral precipitation. Quantitatively, however, the differences in sealing conditions are significant and are typically attributed to differences in experimental conditions or model assumptions. Here we examine the sensitivity of our model, describing CO 2 leakage through wellbores, to cement composition, brine concentration, diffusion rates, and reaction rates. We also evaluate the impact of the boundary condition to allow comparisons between observations from experiments performed at constant flow rate and model predictions made at constant pressure conditions. Our results show that diffusion and reactions rates have the most impact on the self-sealing criteria for cement-CO 2 systems. In addition, conditions associated with self-sealing of fractures at constant flow rate require longer fractures, smaller fracture apertures, and slower velocities than under constant pressure.

58 GEOSCIENCES↗
DOE OSTI2019

Direct in-situ observation of early age void evolution in sustainable cement paste containing fly ash or limestone

This paper uses fast X-ray Computed Tomography (fCT) to study the change in air-filled voids during hydration of portland cement pastes of different water to cement ratios and with fly ash and limestone additives between 30 min and 12 h of hydration with deionized and de-aired water. For the deionized samples, the total volume of the air-filled voids increased during the induction period and decreased as the acceleration period began and finally stayed constant. The samples with 20% replacement of fly ash and 20% replacement of limestone showed the same trends as the OPC samples but with a reduction in the observed air-filled void formation. The air-filled void distribution in these samples changed from a limited number of large voids at the beginning of the measurements to a system with a significantly greater number of uniformly distributed smaller voids. The changes in the air-filled voids were not significant in pastes made with 50% fly ash or with de-aired water in the same testing condition. This might be explained by differences in pore solution chemistry and a reduced amount of dissolved air in the mixing water. A mechanism is proposed for a change in ionic concentration in solution to cause release of the dissolved air within the mixing water.

Cement hydration↗
DOE OSTI2018

Optimal Pre-hydration Age for CO 2 Sequestration through Portland Cement Carbonation

An emerging technology of CO 2 sequestration in Portland cement (PC) is through accelerated carbonation, where PC is intentionally carbonated at early hydration age and reinitiates long-term hydration upon completion of carbonation. However, the current literature has overlooked a fact that different PC hydration ages prior to carbonation (pre-hydration) could lead to distinct carbonation efficiencies and subsequent hydration behaviors (post-hydration). Here, we examine the effects of length of pre-hydration period on CO 2 uptake and on the hydration extent and final strength at 28 days. The CO 2 and H 2 O profiles in the carbonated PC were examined with thermogravimetric analysis/derivative thermogravimetric analysis. The pre-hydration path was traced with isothermal calorimetry. Experimental results suggested that extension of pre-hydration decreased CO 2 uptake, but enhanced the extent of PC hydration at 28 days. It was found that a pre-hydration beyond the late deceleration period of PC hydration (where heat generation is slowing down) led to a higher hydrate content of cement paste, hence forming a higher compressive strength of mortar compared to the noncarbonated benchmarks at 28 days. The lesser carbonation-induced water loss and the nucleation seeding enabled by calcium carbonate are likely responsible for this effect. Furthermore, the finding reported here should be useful for fine tuning PC carbonation process for CO 2 sequestration in concrete.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The Importance of Vane Configuration on Yield Stress Measurements of Cement Slurry

Vane methods combined with direct shear tests are widely applied to measure the yield stress $τ_0$ in concentrated suspensions such as cement slurries. This report reviews three different vanes with different shapes and sizes, and examines the relationship between the yield stress versus the torque and the shear rate versus the angular velocity. This research shows that vanes with conical shapes or reduced height/diameter ratio $(H/D)$ result in larger yield stress values.

36 MATERIALS SCIENCE↗