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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 1,747 records · Page 97
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Acoustic emission Bayesian source location: Onset time challenge

Robust identification of the most accurate observed input data among a pool of observations is key in modeling and decision making. A statistically biased observed measurement deteriorates the predictive power of a model and affects decision-making ability based on the prediction of the model. When two competing methods of measurement are available, such as methods which identify arrival times in acoustic emission (AE) signals, a principal question is whether one of the two obtained datasets, or a combination of the two, should be used later on, for example, to localize an AE source. This question becomes more important when collecting not repeatable data such as AE signals created by a propagating crack. Here this paper considers an inverse source location problem in a concrete block to address the mentioned issue, a proposed methodology which also has wider application in competitive data selection. Elastic energy released by an AE event, such as a propagating crack, is recorded by acoustic emission data acquisition system. The onset time of AE signals is often used to locate the source of the event, and its accuracy directly affects the precision of source identification. This research proposes an innovative approach to select the most probable onset time obtained from two automatic picker methods. The proposed method selects the most probable onset times, which are observed by each picker for each sensor, in a probabilistic fashion. To validate the proposed method, the most accurate onset time observed by each picker is identified by visual inspection and is compared with the one is selected by the proposed method. Finally, the dataset is used for source location identification. Results show that picked onset times determined by the proposed method generate more accurate source identification when compared with coordinates obtained using each dataset individually.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

The gyrokinetic field invariant and electromagnetic temperature-gradient instabilities in ‘good-curvature’ plasmas

Curvature-driven instabilities are ubiquitous in magnetised fusion plasmas. By analysing the conservation laws of the gyrokinetic system of equations, we demonstrate that the well-known spatial localisation of these instabilities to regions of ‘bad magnetic curvature’ can be explained using the conservation law for a sign-indefinite quadratic quantity that we call the gyrokinetic field invariant. Its evolution equation allows us to define the local effective magnetic curvature whose sign demarcates the regions of ‘good’ and ‘bad’ curvature, which, under some additional simplifying assumptions, can be shown to correspond to the inboard (high-field) and outboard (low-field) sides of a tokamak plasma, respectively. We find that, given some reasonable assumptions, electrostatic curvature-driven modes are always localised to the regions of bad magnetic curvature, regardless of the specific character of the instability. More importantly, we also deduce that any mode that is unstable in the region of good magnetic curvature must be electromagnetic in nature. As a concrete example, we present the magnetic-drift mode, a novel good-curvature electromagnetic instability, and compare its properties with the well-known electron-temperature-gradient instability. Finally, we discuss the relevance of the magnetic drift mode for high-β fusion plasmas, and in particular its relationship with microtearing modes.

fusion plasma↗
DOE OSTI2020

Numerical methods for nonlocal and fractional models

Partial differential equations (PDEs) are used with huge success to model phenomena across all scientific and engineering disciplines. However, across an equally wide swath, there exist situations in which PDEs fail to adequately model observed phenomena, or are not the best available model for that purpose. On the other hand, in many situations, nonlocal models that account for interaction occurring at a distance have been shown to more faithfully and effectively model observed phenomena that involve possible singularities and other anomalies. Here, we consider a generic nonlocal model, beginning with a short review of its definition, the properties of its solution, its mathematical analysis and of specific concrete examples. We then provide extensive discussions about numerical methods, including finite element, finite difference and spectral methods, for determining approximate solutions of the nonlocal models considered. In that discussion, we pay particular attention to a special class of nonlocal models that are the most widely studied in the literature, namely those involving fractional derivatives. The article ends with brief considerations of several modelling and algorithmic extensions, which serve to show the wide applicability of nonlocal modelling.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Nanoparticle Tracking to Probe Transport in Porous Media

From the granular and fractured subsurface environment to highly engineered polymer membranes used in pharmaceutical purification, porous materials are ubiquitous in nature and industrial applications. In particular, porous media are used extensively in processes including water treatment, pharmaceutical sterilization, food/beverage processing and heterogeneous catalysis, where hindered mass transport is either essential to the process or a necessary, but undesirable limitation. Unfortunately, there are currently no universal models capable of predicting mass transport based on a description of the porous material because real porous materials are complex, and because many coupled dynamic mechanisms (e.g. adsorption, steric effects, hydrodynamic effects, electrostatic interactions, etc.) give rise to the observed macroscopic transport phenomena. While classical techniques, like nuclear magnetic resonance and dynamic light scattering, provide useful information about mass transport in porous media at the ensemble level, they provide limited insight into the microscopic mechanisms that give rise to complex phenomena such as anomalous diffusion, hindered pore-space accessibility, and unexpected retention under flow, among many others. To address this issue, we have developed refractive index matching imaging systems, combined with single-particle tracking methods, allowing the direct visualization of single particle motion within a variety of porous materials. Here, we summarize our recent efforts to advance the understanding of nanoparticle transport in porous media using single-particle tracking methods in both fundamental and applied scenarios. First, we describe the basic principles for two-dimensional and three-dimensional single-particle tracking in porous materials. Then, we describe concrete examples of nanoparticle transport in porous materials from two perspectives: (1) understanding fundamental elementary particle transport processes in porous media, including pore accessibility and cavity escape, which limit transport in porous media; (2) facilitating applications in industrial processes, e.g. by understanding the mechanisms of particle fouling and remobilization in filtration membranes. Finally, we provide an outlook of opportunities associated with investigating other types of mass transport in confined environments using single-particle tracking methods, including electrophoretic and self-propelled motion.

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

Design Principles for Efficient and Stable Water Splitting Photoelectrocatalysts

Photoelectrochemical water splitting is a promising avenue for sustainable production of hydrogen used in the chemical industry and hydrogen fuel cells. The basic components of most photoelectrochemical water splitting systems are semiconductor light absorbers coupled to electrocatalysts, which perform the desired chemical reactions. A critical challenge for the design of these systems is the lack of stability for the majority of desired semiconductors under operating water splitting conditions. One strategy to address this issue is to protect the semiconductor by covering it with a stabilizing insulator layer, creating a metal–insulator–semiconductor (MIS) architecture, which has demonstrated improved stability. In addition to enhanced stability, the insulator layer may significantly affect the electron and hole transfer, which governs the recombination rates. Furthermore, the insertion of an insulator layer leads to the introduction of additional insulator/electrocatalyst and insulator/semiconductor interfaces. These interfaces can impact the system’s performance significantly, and they need to be carefully engineered to optimize the efficiencies of MIS systems. In this Account, we describe our recent progress in shedding light on the critical role of the insulator and the interfaces on the performance of MIS systems. We discuss our findings by focusing on the concrete example of planar n-type Si protected by a HfO 2 insulator layer and coupled to a Ni or Ir electrocatalyst that performs the oxygen evolution reaction, one of the water splitting half-reactions. To improve our fundamental understanding of the insulator layer, we precisely control the HfO 2 insulator thickness using atomic layer deposition (ALD), and we perform a series of rigorous electrochemical experiments coupled with theory and modeling. We demonstrate that by tuning the insulator thickness, we can control the flux and recombination of photogenerated electrons and holes to optimize the generated photovoltage. Despite optimizing the thickness, we find that the maximum generated photovoltage in MIS systems is often significantly lower than the upper performance limit, i.e., there are additional losses in the system that could not be addressed by optimizing the insulator thickness. We identify the sources of these losses and describe strategies to minimize them by a combination of improving the semiconductor light absorption, removing nonidealities associated with interfacial defects, and finding alternative insulators with improved charge carrier selectivity. Finally, we quantify the improvements that can be obtained by implementing these specific strategies. Our collective work outlines strategies to analyze MIS systems, identify the sources of efficiency losses, and optimize the design to approach the fundamental performance limits. Furthermore, these general approaches are broadly applicable to photoelectrochemical materials that utilize sunlight to produce value-added chemicals.

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

Pressure-Sensitive Adhesive Combined with Paper Spray Mass Spectrometry for Low-Cost Collection and Analysis of Drug Residues

Illicit drug use causes over half a million deaths worldwide every year. Drugs of abuse are commonly smuggled through customs and border checkpoints and, increasingly, through parcel delivery services. Improved methods for detection of trace drug residues from surfaces are needed. Such methods should be robust, fieldable, sensitive, and capable of detecting a wide range of drugs. In this work, commercially produced paper with a pressure-sensitive adhesive coating was utilized for the collection and analysis of trace drug residues by paper spray mass spectrometry (MS). This modified substrate was used to combine sample collection of drug residues from surfaces with rapid detection using a single paper spray ticket. The all-in-one ticket was used to probe different surfaces commonly encountered in forensic work including clothing, cardboard, glass, concrete, asphalt, and aluminum. A total of 10 drugs (acetyl fentanyl, fentanyl, clonazolam, cocaine, heroin, ketamine, methamphetamine, methylone, U-47700, and XLR-11) were evaluated and found to be detectable in the picogram range using a benchtop mass spectrometer and in the low nanogram range using a portable ion trap MS. Finally, the novel approach demonstrates a simple yet effective sampling strategy, allowing for rapid identification from difficult surfaces via paper spray mass spectrometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Mechanistic Studies of Chain Termination and Monomer Absorption in Molecular Layer Deposition

Here, molecular layer deposition (MLD) is of growing interest as a vapor-phase method for depositing ultrathin polymeric films. The amount of material deposited per cycle of MLD is believed to be strongly dependent on the number of available surface reaction sites. However, the factors that alter the number of reactive sites during cycling have not been well understood. In this work, we provide concrete evidence that although chain termination reactions may reduce the number of reaction sites, the adsorption or absorption of monomers allows for the introduction of new reaction sites. These absorbed monomers are strongly bound to the film and allow the films to recover from growth defects introduced by chain terminations. A mathematical model for growth is developed and suggests that these absorptions eventually lead to the characteristic steady-state growth rate seen for MLD processes. Fits of the model to the experimental data for polyurea MLD indicate that ~3% of the chains experience termination events during each cycle at steady state, with any given chain having an ≈50% chance to be terminated before reaching 22 cycles; this termination is then compensated for by uptake of new monomers. Together, these results indicate that typical MLD growth involves the continuous occurrence of termination reactions and the renucleation of chains within the film via the absorption of monomers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Process Modeling and Techno-Economic Analysis of a CO 2 Capture Process Using Fixed Bed Reactors with a Microencapsulated Solvent

A detailed model of a capsule containing sodium carbonate solution is developed here to study the microencapsulated carbon capture solvents (MECS). A rigorous vapor–liquid equilibrium model is developed for the Na 2 CO 3 –CO 2 –H 2 O system, where liquid-phase nonideality is modeled by the electrolyte nonrandom two-liquid model. The data from the experiments conducted at the Lawrence Livermore National Laboratory is used to obtain a maximum likelihood estimate of the initial solvent concentration inside the capsules and the parameters for the capsule model. A nonisothermal, dynamic model of a fixed bed contactor filled with these capsules is then developed. In addition to direct steam injection, indirect heating using an embedded heat exchanger is modeled for desorption. Finally, the model is used to simulate temperature swing absorption and desorption cycles. The results of these studies indicate that there is an optimal residence time or superficial flue gas velocity to minimize the bed volume. However, the total energy requirement for desorption monotonically decreases with increased residence time as the proportion of the sensible heat to the total regeneration heat keeps decreasing. Furthermore, heat recovery from the bed is crucial to keep energy penalty for regeneration low. A techno-economic analysis is conducted, and the equivalent annual operating cost (EAOC) is analyzed for two different reactor materials (concrete and carbon-steel) and compared with a system using a conventional monoethanolamine (MEA) solvent. In this work, the minimum EAOC for the MECS fixed bed configuration is approximately 1.8–2.7 times higher than the EAOC for an MEA system with a similar amount of heat recovery (85%). The impact of ±50% uncertainty in the capital cost estimate is also evaluated, and the minimum EAOC is 1.5 times higher than the MEA technology for 85% heat recovery. These results using microencapsulated sodium carbonate solution are a starting point that sets an upper limit on the cost of the MECS carbon-capture system. Improvements to the MECS capsules (e.g., using a higher carbonate concentration and lowering the shell mass transfer resistance) and also exploring other contactor technologies are expected to decrease the system cost and make it more competitive.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2025

Greenhouse Gas Emissions and Decarbonization Potential of Global Fired Clay Brick Production

Fired clay bricks (FCBs) are a dominant building material globally due to their low cost and simplicity of production, especially in low- and middle-income countries. With a projected rising housing demand, commensurate growth in brick demand is anticipated, the production of which could result in significant greenhouse gas (GHG) emissions. Robust models are needed to estimate brick demand and emissions to systematically address decarbonization pathways. Few sources report production values; hence, we present two novel proxy models: (i) a consumption prediction model, relying on country-specific clay extraction data, dynamic building stock modeling, and average material intensity use allowing for projections to 2050; and (ii) a GHG emissions model, using literature-based data and production technology-specific inputs. Based on these models, the current global FCB consumption is estimated as 2.18 Gt annually, resulting in approximately 500 million tCO2e (1% of current global GHG emissions). If unaddressed, this fraction could increase to 3.5-5% in 2050 considering a moderate SSP 2-4.5 climate change mitigation scenario. Consequently, we explored three potential decarbonization pathways: (i) improving energy efficiency; (ii) shifting production to best practices; and (iii) replacing half of FCB demand with hollow concrete blocks, resulting in 27%, 49%, and 51% reduction in GHG emissions, respectively.

Olsson, Josefine A↗
DOE OSTI2025

Predictive Assessment of the Chemical Composition of Coal Ash in Reserve at U.S. Disposal Sites

In the United States, more than 2 Gt of coal combustion residuals (i.e., coal ash) are stored in hundreds of disposal units. Recent federal regulations mandate the closure or retrofitting of most coal ash impoundments, presenting significant challenges for waste management. These regulatory pressures also present opportunities to reuse coal ash. However, the quality and quantity of discarded coal ash across the U.S. are not well known, even though this information is crucial for spurring its reuse for conventional and new material applications. This study describes a predictive model for the major element composition of coal ash in reserve at disposal sites of major U.S. coal-fired power plants. This model was constructed from coal purchase records of 705 power stations from 1973 to 2022 and was trained on coal ash composition data, showing that coal ash elemental composition is strongly associated with the source of feedstock coal. The model showed regional shifts in the major element contents of ash produced by power plants in the last 50 years, particularly for calcium and iron (expressed as %CaO and %Fe2O3), as power stations changed their source of coal over this time frame. Our approach enables an estimation of chemical composition for ash stored in waste impoundments at individual power stations. Such information can help to delineate the regional market resource potential of supplementary cements for concrete and other material innovations that would utilize coal ash harvested from disposal sites across the U.S.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2019

Quantifying the Impact of Magnesium on the Stability and Water Binding Energy of Hydrated Calcium Carbonates by ab initio Thermodynamics

Determining conditions that drive carbonate formation is important for establishing paleoindicators for mineral deposition, understanding the carbon cycle and biomineralization, and designing industrial applications such as scale inhibition, manufacturing of cement and concrete, and environmental remediation. Mg and incorporated water have been observed to play critical roles in nonclassical crystallization pathways of calcium carbonate, the dominant carbonate found in nature, through promoting formation of low energy metastable intermediates such as monohydrocalcite (CaCO3H2O), ikaite (CaCO36H2O), and amorphous calcium carbonate (CaCO3H2O). The impact of Mg on the thermodynamics and water binding ability of these hydrated intermediates is challenging to measure and is not understood at the molecular level. In this work density-functional theory and ab initio thermodynamics are used to quantify the impact of Mg on structure, thermodynamics and water binding energies of the crystalline hydrated Ca carbonates as a function of temperature in aqueous and ultra-high vacuum conditions, as well as CO2-rich environments relevant to carbon sequestration. For monohydrocalcite, Mg incorporation is found to destabilize the structure despite a dramatic increase in the water-binding energy, thus confirming that Mg promotes monohydrocalcite formation kinetically rather than thermodynamically. For ikaite, however, Mg promotes its formation both kinetically and thermodynamically, expanding the stability region for ikaite in cold water. For portlandite Ca(OH)2, Mg significantly destabilizes the structure which cannot shift atomic positions to accommodate the smaller cation, unlike the positional flexibility afforded by water molecules and carbonate groups in monohydrocalcite and ikaite. Mg does result in a decreased lattice volume for ikaite and monohydrocalcite, but only a very small amount and hence cannot be used to quantify the amount of Mg incorporation in natural samples.

calcite, ikaite, monohydrocalcite, magnesium, carb↗
DOE OSTI2016

Dissociation of sarin on a cement analogue surface: Effects of humidity and confined geometry

Here, first-principles molecular dynamics simulations were used to investigate the dissociation of sarin (GB) on the calcium silicate hydrate (CSH) mineral tobermorite (TBM), a surrogate for cement. CSH minerals (including TBM) and amorphous materials of similar composition are the major components of Portland cement, the binding agent of concrete. Metadynamics simulations were used to investigate the effect of the TBM surface and confinement in a microscale pore on the mechanism and free energy of dissociation of GB. Our results indicate that both the adsorption site and the humidity of the local environment significantly affect the sarin dissociation energy. In particular, sarin dissociation in a low-water environment occurs via a dealkylation mechanism, which is consistent with previous experimental studies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Quantification of Deformation-Induced Concentration Fluctuations in Polymeric Liquids by Small-Angle Neutron Scattering

This study demonstrates how the large concentration fluctuations of polymeric liquids under deformation and flow can be quantitatively studied by applying the spherical harmonic expansion technique to small-angle neutron scattering. Using a series of binary polymer blends, it is shown that the emergence of the so-called butterfly patterns is caused by the change of sign in the leading anisotropic component of the small-angle spectrum, when the scattering is dominated by intermolecular correlation associated with flow-induced demixing. The increasing spatial fluctuations of concentration are evidenced by the enhancement of the isotropic component of the scattering spectrum in the zero-angle limit and peak shift of the leading anisotropic coefficients toward low Q. Additionally, the spherical harmonic expansion framework permits real-space analysis of anisotropic scattering length density correlation in a convenient form. The methodology described in this work provides a concrete venue for quantitative studies of phase behavior of fluids under deformation and flow via small-angle scattering techniques, where mainly qualitative approaches were previously employed.

Chemical structure↗
DOE OSTI2016

Confined Water in Layered Silicates: The Origin of Anomalous Thermal Expansion Behavior in Calcium-Silicate-Hydrates

Water, under conditions of nanoscale confinement, exhibits anomalous dynamics, and enhanced thermal deformations, which may be further enhanced when such water is in contact with hydrophilic surfaces. Such heightened thermal deformations of water could control the volume stability of hydrated materials containing nanoconfined structural water. Understanding and predicting the thermal deformation coefficient (TDC, often referred to as the CTE, coefficient of thermal expansion), which represents volume changes induced in materials under conditions of changing temperature, is of critical importance for hydrated solids including: hydrogels, biological tissues, and calcium silicate hydrates, as changes in their volume can result in stress development, and cracking. By pioneering atomistic simulations, we examine the physical origin of thermal expansion in calcium-silicate-hydrates (C–S–H), the binding agent in concrete that is formed by the reaction of cement with water. We report that the TDC of C–S–H shows a sudden increase when the CaO/SiO 2 (molar ratio; abbreviated as Ca/Si) exceeds 1.5. This anomalous behavior arises from a notable increase in the confinement of water contained in the C–S–H’s nanostructure. We identify that confinement is dictated by the topology of the C–S–H’s atomic network. Altogether, the results suggest that thermal deformations of hydrated silicates can be altered by inducing compositional changes, which in turn alter the atomic topology and the resultant volume stability of the solids.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Direct-Write 3D Nanoprinting of Plasmonic Structures

During the past decade, significant progress has been made in the field of resonant optics ranging from fundamental aspects to concrete applications. And while several techniques have been introduced for the fabrication of highly defined metallic nanostructures, the synthesis of complex, free-standing three-dimensional (3D) structures is still an intriguing, but so far intractable, challenge. Here, we demonstrate a 3D direct-write synthesis approach that addresses this challenge. Specifically, we succeeded in the direct-write fabrication of 3D nanoarchitectures via electron-stimulated reactions, which are applicable on virtually any material and surface morphology. Furthermore, by that, complex 3D nanostructures composed of highly compact, pure gold can be fabricated, which reveal strong plasmonic activity and pave the way for a new generation of 3D nanoplasmonic architectures that can be printed on-demand.

36 MATERIALS SCIENCE↗
DOE OSTI2020

High-Performance Thermoelectric Generators for Field Deployments

Thermoelectric power generation is a reliable energy harvesting technique for directly converting heat into electricity. Recent studies have reported the thermal-to-electrical energy conversion efficiency of thermoelectric generators (TEGs) up to 11% under laboratory settings. However, the practical effectiveness of TEGs deployed under real environments is still not more than a few percent. In this study, we provide fundamental insight on the operation of TEGs in realistic environments by illustrating the combinatory effect of thermoelectric material properties, device boundary conditions, and environmental thermal resistivity on TEG performance in conjunction with the module parameters. Using numerical and experimental studies, we demonstrate the existence of a critical heat transfer coefficient that dramatically affects the design and performance of TEGs. Results provide a set of concrete design criteria for developing efficient TEGs that meet the metrics for field deployments. High-performance TEGs demonstrated in this study generated up to 28% higher power and 162% higher power per unit mass of thermoelectric materials as compared to the commercial module deployed for low-grade waste heat recovery. This advancement in understanding the TEG operation will have a transformative impact on the development of scalable thermal energy harvesters and in realizing their practical targets for efficiency, power density, and total output power.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
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 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↗