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At least 937 records · Page 52
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

The impact of carbonation on bulk and ITZ porosity in microconcrete materials with fly ash replacement

Scanning electron microscopy was used to evaluate the porosity patterns found in microconcrete materials to better understand the gaseous diffusion pathways and reaction of CO{sub 2} within the bulk cement paste and interfacial transition zone (ITZ) of microconcrete materials containing different fly ash replacement types. Image segmentation was applied to evaluate the porosity as a function of distance from an exposed surface in the bulk cement paste and from aggregate boundaries in the ITZ in both carbonated and non-carbonated microconcrete materials. The ITZ region remained more porous compared to the bulk cement paste for all microconcrete types after carbonation despite a change in the porosity profile across the ITZ region. Results indicate that both the carbonation reaction capacity and porosity before carbonation impact the decrease in porosity observed as a result of carbonation in the ITZ and bulk cement paste regions.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Estimating the mechanical properties of hydrating blended cementitious materials: An investigation based on micromechanics

The hydration model of Parrot & Killoh (1984) has been extended to blended cements and coupled to a micromechanical scheme similar to that of Pichler & Hellmich (2011) to estimate the Young modulus and the compressive strength of cementitious materials as a function of time. A finite aspect ratio of 7 is introduced to describe the shape of the hydrates and improve the estimate of the early age strength by the micromechanical scheme. Furthermore, accounting for the stress fluctuations in the cement paste partly explains the fact that the compressive strength of a concrete can be lower than that of its cement paste. Finally, the estimated physical properties are compared to numerous experimental measurements from the literature and new experimental measurements on blended cement pastes featuring significant weight fractions of limestone filler, fly ash or silica fume. It is shown that the present model slightly overestimates the dilution effect.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Effect of fly ash microsphere on the rheology and microstructure of alkali-activated fly ash/slag pastes

Highlights: • Fly ash microsphere is collected from fly ash with electrostatic adsorption classification. • Fly ash microsphere acts as 'ball-bearings' in alkali-activated cements. • Fly ash microsphere works as inorganic dispersing agent to improve workability. • Fly ash microsphere exhibits a good compatibility in alkali-activated cements. - Abstract: The highly viscous property of alkali silicate-activated cements is one of the critical challenges that hinder their wide application. The present study focuses on ameliorating the rheological performance of sodium silicate-activated fly ash/slag pastes by using fly ash microsphere (FAM), which are highly spherical particles collected from fly ash with electrostatic adsorption classification technology. The FAM particles work as 'ball-bearings' in the pastes to reduce the internal friction between fly ash and slag grains, and meanwhile mitigate the agglomeration of flocs and fragmentation to release the locked water. The interrelationship between the FAM particle geometry and plastic viscosity of the paste is well described by the Krieger-Dougherty equation, which supports the proposed mechanisms of 'ball-bearings' effects. FAM can work as an inorganic dispersing agent to improve the workability of alkali-activated cement products for a variety of application aspects.

36 MATERIALS SCIENCE↗
DOE OSTI2018

C–S–H gel densification: The impact of the nanoscale on self-desiccation and sorption isotherms

The relationship between humidity and water content in a hydrating cement paste is largely controlled by the nanostructure of the C–S–H gel. Current hydration models do not describe this nanostructure, thus sorption isotherms and self-desiccation are given as constitutive inputs instead of being predicted from microstructural evolution. To address this limitation, this work combines a C–S–H gel description from nanoscale simulations with evolving capillary pore size distributions from a simple hydration model. Results show that a progressive densification of the C–S–H gel must be considered in order to explain the self-desiccation of low-alkali pastes. The impact of C–S–H densification on the evolution of microstructure and sorption isotherms is then discussed, including the effect of water-to-cement ratio, cement powder fineness, and curing temperature. Overall, this work identifies an area where nanoscale simulations can integrate larger-scale models of cement hydration and poromechanics.

36 MATERIALS SCIENCE↗
DOE OSTI2018

The synthesis and hydration of ternesite, Ca5(SiO4)2SO4

The hydration and strength evolution of two multi-phase ternesite-based cements with 15 and 29 wt% ternesite are reported. The synthesis and hydration properties of single phase ternesite, nominally Ca{sub 5}(SiO{sub 4}){sub 2}SO{sub 4}, are also reported including both chemically-pure ternesite and preparations doped with sodium, potassium, phosphorous, magnesium, manganese, strontium, zinc and titanium oxides. Hydration of the samples at 25 °C was studied by calorimetry and quantitative X-ray diffraction. Unconfined compressive strength development was determined for up to 1 year. Single-phase chemically activated ternesite hydrated rapidly at 25 °C achieved compressive strengths of ≈30 and ≈65 MPa at 28 and 90 days respectively, with C-S-H and gypsum as hydration products. The multi-phase ternesite-based cements reached 7 day strengths of ≈30 MPa. It is concluded that ternesite reacts with water, exhibiting strength gain. The future of calcium sulfoaluminate and sulfosilicate cements is discussed and it is suggested that a considerable, and as yet unrealised scope exists for simultaneously optimising cementing properties while lowering production costs and reducing CO{sub 2} emissions.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effects of organic additives on calcium hydroxide crystallisation during lime slaking

Highlights: • Sucrose and lignosulfonate reduce the crystallite size of Ca(OH){sub 2}. • Lime slaking in sucrose solutions leads to Ca(OH)2 with irregular shape. • Lime slaking in presence of lignosulfonate leads to plate-like Ca(OH){sub 2} crystals. • Effects of additives are enhanced when introduced before slaking. • Additives stabilise the unstable edge faces of Ca(OH){sub 2} during ageing. Organic compounds, often used in cement systems as admixtures, may affect the crystallisation and carbonation kinetics of Ca(OH){sub 2}, an important phase of hydrated cement. Here, we investigated changes in Ca(OH){sub 2} morphology in the presence of 3 organic compounds, commonly encountered in cement and lime-based materials: sucrose, pectin and calcium lignosulfonate. The additives were introduced either before or after lime slaking to determine the influence of temperature. Ca(OH){sub 2} crystals and supernatant solutions were characterised at time of slaking and after 6 months of ageing using scanning electron microscopy, X-ray diffraction and optical emission spectroscopy. Our results indicate that the morphology of Ca(OH){sub 2} crystals is modified by the characteristics of the organic molecules which promote formation of Ca(OH){sub 2} with habits that can result in faster carbonation, an effect that is detrimental to cement used in reinforced concrete. These effects are enhanced when the additives are introduced before slaking, likely as a result of thermal degradation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Estimating viscoelastic compliance of desiccating cementitious materials using drying prism tests

Highlights: • Determining relative humidity and degree of reaction of desiccating cementitious materials via an integrated method • Extracting moisture diffusion coefficient of cement mortar using the mass loss data of the prism specimens • Estimating uniaxial viscoelastic compliance of cement mortar using the shrinkage strain data of the prism specimens An integrated modeling approach to determining internal relative humidity and degree of reaction of desiccating cementitious materials has been developed. By simultaneously accounting for both self-desiccation and external drying, the model is capable of predicting the evolution of material properties of desiccating cementitious materials. Using the mass loss data of the prism specimens, the moisture diffusion coefficient of a nonlinear model for cement mortar was determined. Additionally, a previous poroviscoelastic shrinkage model was modified and extended. Through comparison of predicted and measured axial strain of the prism specimens, the viscoelastic compliance of cement mortar was extracted. The present work revealed that it is possible to use a simple drying prism test to fit the moisture diffusion coefficient and creep compliance of cementitious materials, though the comparison of the extracted viscoelastic compliance with measured compliance was only reasonable if the outer layer of the drying mortar was presumed to have microcracking.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Factors affecting the reactivity of slag at early and late ages

This study investigates the difference between the reactivity of slag in NaOH solution (w/s = 100) and in cement paste (w/b = 0.4). The reactivity of slag is much higher in NaOH solution than in cement paste. When the NaOH solution is saturated with portlandite, the rate of reaction of slag decreases to approach that in cement paste. This suggests that the slower reaction of slag in cement paste might be due to the presence of calcium ions released by the clinker phases. At 28 days, relative humidity measurements indicate that water is only present in pores less than 6 nm. Above 6 nm, hydration cannot take place due to the lack of water. From a thermodynamic point of view, the small size of water filled pores may slow down the slag reaction due to the high concentration of species in solution required for hydrate growth to balance the increase of the surface energy.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Drying shrinkage of alkali activated binders cured at room temperature

Alkali activated binders tend to exhibit higher drying shrinkage movements when compared with Portland cement. An experimental investigation was undertaken in order to assess the drying shrinkage of a basic alkali activated binder versus Portland cement, and to evaluate the effectiveness of different additives in reducing the drying shrinkage of the alkali activated binder. The results indicated that the drying shrinkage of the basic alkali activated binder was about twice that of Type I Portland cement. Some of the additives used to refine the alkali activated binder formulation were found to lower the drying shrinkage of the alkali activated binder to levels that were comparable with that of Portland cement. Explanations were presented for the mechanisms through which these additives enhance the dimensional stability of the alkali activated binder. SEM, TG/DTG and heat of hydration techniques were used to gain more insight into the mechanisms of action of different additives in alkali activated binders.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Irradiated recycled plastic as a concrete additive for improved chemo-mechanical properties and lower carbon footprint

Concrete production contributes heavily to greenhouse gas emissions, thus a need exists for the development of durable and sustainable concrete with a lower carbon footprint. This can be achieved when cement is partially replaced with another material, such as waste plastic, though normally with a tradeoff in compressive strength. This study discusses progress toward a high/medium strength concrete with a dense, cementitious matrix that contains an irradiated plastic additive, recovering the compressive strength while displacing concrete with waste materials to reduce greenhouse gas generation. Compressive strength tests showed that the addition of high dose (100 kGy) irradiated plastic in multiple concretes resulted in increased compressive strength as compared to samples containing regular, nonirradiated plastic. This suggests that irradiating plastic at a high dose is a viable potential solution for regaining some of the strength that is lost when plastic is added to cement paste. X-ray Diffraction (XRD), Backscattered Electron Microscopy (BSE), and X-ray microtomography explain the mechanisms for strength retention when using irradiated plastic as a filler for cement paste. By partially replacing Portland cement with a recycled waste plastic, this design may have a potential to contribute to reduced carbon emissions when scaled to the level of mass concrete production.

42 ENGINEERING↗
DOE OSTI2017

Ca L 2,3 -edge near edge X-ray absorption fine structure of tricalcium aluminate, gypsum, and calcium (sulfo)aluminate hydrates

Tricalcium aluminate (cement clinker phase), gypsum, katoite, ettringite, and calcium monosulfoaluminate hydrate (abbreviated as kuzelite) are the major minerals in the hydration reaction of tricalcium aluminate in the presence of gypsum and have critical impacts on the kinetics and thermodynamics of early-age cement hydration mechanisms. In this paper, spectroscopic analysis of these minerals is conducted using scanning transmission X-ray microscopy (STXM). Their Ca L 2,3 -edge near edge X-ray absorption fine structure (NEXAFS) spectra are measured and correlated to the known Ca coordination environments. The results indicate that these minerals have unique Ca environments that can be differentiated from one another based on the intensities and positions of the absorption peaks at 346.5–348.5 and 350.5–351.5 eV. It is concluded that Ca in tricalcium aluminate (cubic and orthorhombic polymorphs) and katoite is in cubic-like coordination with negative 10Dq, whereas Ca is in an octahedral-like coordination with positive 10Dq in ettringite, gypsum, and kuzelite. For tricalcium aluminate, the Ca atoms in both polymorphs are in similar chemical environments with slightly more distortion in the orthorhombic polymorph. As a common issue in STXM experiments, absorption saturation of NEXAFS spectra is also investigated. It is demonstrated that the optical density difference between pre- and post-edge absorption levels provides a reliable indication of the sample thickness in the systems studied. Finally, the present work provides a reference for the STXM study of the calcium (sulfo)aluminate reactions in cement hydration and natural aqueous environments, and in the former case, provides a more complete understanding of a system that may serve as a low-C alternative to Portland cement.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Development of Magnesium Oxysulfate Formulation for SRPPF Aqueous Recovery Liquid Solidification

The liquid effluent from the Savannah River Plutonium Processing Facility (SRPPF) Aqueous Recovery Processes will be solidified into a stable form that is acceptable by Waste Isolation Pilot Plant (WIPP) for disposal. The current Aqueous Recovery flow sheet proposes to solidify the liquid effluent using a grout formula that was developed and tested for the former Waste Solidification Building process. This Portland cement based mixture results in a high pH (~13) leachate from the solidified waste form which is not acceptable to WIPP in the large quantities expected from production at SRPPF. Various cementitious materials were previously evaluated as alternative grout formulations to Portland cement and a MgO-based mix was identified as a promising alternative. A magnesium oxysulfate (MOS) cement formulation comprised of reactive magnesium oxide (MgO), anhydrous magnesium sulfate (MgSO 4 ), and sand, as a non-reactive heat sink provided good mixability, similar density to the original Portland-cement based mix, and a leachate pH of 9.4, within the assumed WIPP brine pH range. However, the MOS formulation exhibited an appreciable amount of heat generation, which resulted in premature setting of a large-scale test.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Municipal Solid Waste Incineration Ash-Incorporated Concrete: One Step towards Environmental Justice

Municipal solid waste and cement manufacture are two sources of environmental justice issues in urban and suburban areas. Waste utilization is an attractive alternative to disposal for eliminating environmental injustice, reducing potential hazards, and improving urban sustainability. The re-use and recycling of municipal solid waste incineration (MSWI) ash in the construction industry has drawn significant attention. Incorporating MSWI ash in cement and concrete production is a potential path that mitigates the environmental justice issues in waste management and the construction industry. This paper presents a critical overview of the pretreatment methods that optimize MSWI ash utilization in cement/concrete and the influences of MSWI ash on the performance of cement/concrete. This review aims to elucidate the potential advantages and limitations associated with the use of MSWI ash for producing cement clinker, alternative binder (e.g., alkali-activated material), cement substitutes, and aggregates. A brief overview of the generation and characteristics of MSWI ash is reported, accompanied by identifying opportunities for the use of MSWI ash-incorporated products in industrial-scale applications and recognizing associated environmental justice implications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Installation and operation of GeoMelt{sup R} in container vitrification in NNL Central Lab active rig hall at Sellafield - 15328

Cleanup and subsequent immobilization of wastes on the UK's NDA estate brings major challenges. With the exception of HLW where vitrification is utilized for immobilization, cement is typically used in the management and immobilization of non-heat generating wastes. However some legacy feeds such as those containing reactive metals can be incompatible with cementation technologies, and the application of engineered cement encapsulating product to raw wastes increases wasteform volume. Cementation has also been developed to be compatible with the repository concept, which provides it with a level of protection from the environment. Potential delays in repository implementation and as yet to be determined repository waste form acceptance criteria for some wastes may require the duration of above ground storage of immobilized wastes to be extended with potential effect on the integrity of the wasteform. Vitrification is a treatment option which destroys organics and hazardous inorganics such as asbestos, reduces wasteform volume, and produces a robust leach resistant wasteform. Kurion's GeoMelt{sup R} In-container Vitrification (ICV){sup TM} is a vitrification process wherein the treatment vessel can serve as an interim-storage, transport, and final long-term storage vessel - thus negating the need to pour glass into a separate container, effectively leading to a much simpler system than traditional waste melters. The inherent volume reduction from vitrification results in a dense product with self-shielding properties, and the GeoMelt treatment process has been demonstrated to homogenize elemental metals and radionuclide contaminants of concern, eliminating hot spots and mitigating criticality concerns. All of which opens up alternatives strategies for storage and disposal. GeoMelt has been proven in the commercial and US DOE waste treatment environment with over 26,000 tonnes of hazardous waste treated to date (half of this radioactive). Kurion and the UK's National Nuclear Laboratory (NNL) plan to demonstrate its application to Sellafield radioactive wastes. A small (engineering) scale demonstrator is being installed in the active rig hall at NNL's Central Laboratory at Sellafield UK with a twofold mission; 1) demonstration of the vitrification of ILW/LLW, and 2) processing of smaller volume orphan wastes that currently have no treatment path. The NNL facility will allow the handling of uranium containing materials which form a substantial component of ILW currently stored on the Sellafield site. Accurate DFs across the melter and off gas system are often difficult to obtain using inactive materials at the low concentrations present in radioactive wastes. Installation in the NNL facility will allow trace quantities of active species such as Cs-137 and Tc-99 to be processed as part of a simulant ILW stream and monitoring will allow accurate decontamination factors (DFs) to be established to support future vitrification facility design. In addition to underpinning melter operation and obtaining DFs across the system, the facility will allow the processing of radioactive waste arisings of low activity which may either be typical of larger waste volumes or may present as orphans without a disposition route. In either case the melter facility will be able to vitrify these wastes into a form that will be suitable for interim storage and disposal. Among the feeds envisaged for processing will be asbestos from power stations, contaminated soils, feeds containing uranium metals, ponds solids, sludge, and miscellaneous active laboratory wastes. The NNL Central Lab capability will be used to analyze the active product to support disposal requirements whether through letters of compliance for the Geological Disposal Facility (GDF) or waste acceptance criteria for the Low Level Waste Repository (LLWR). (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Optimising Blends of Blast Furnace Slag for the Immobilisation of Nuclear Waste - 16245

The legacy of nuclear waste at the Sellafield site in the UK is an ongoing issue, and the current preferred route for the disposal of low and intermediate level waste is encapsulation in a cementitious matrix, formulated by blending Portland cement with blast furnace slag (BFS). Due to demands and economic challenges faced by the cement and steel industries, the supply of BFS to the UK nuclear industry has been inconsistent. These changes have caused the industry to move from a unique BFS powder supply with a certain specification to a combination of standard commercially available cementitious powders. The material currently used at the Sellafield site is a blend of ground granulated blast furnace slag (GGBS) and a coarser fraction of the same composition called Calumite, combined with Portland cement. This work involves future-proofing the supply of BFS for the UK nuclear industry by optimising the blend of the two fractions of BFS in order to replicate the unique specification required by Sellafield Ltd. The main emphasis is on the particle size distribution (PSD) and how this impacts the properties of the final wasteform. The study investigates the performance properties of the blended grouts such as workability, particle packing and heat evolution. Results show that the PSD of the cement powders affect both the physical and chemical properties of the cementitious matrix produced. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Investigating the Depth of Penetration of Radionuclides in Concrete - 16292

This paper focuses on some chemical and structural aspects for mature concrete structural substrate that functions as a barrier to radioactive material migration. Exposure to radioactive material may be a consequence of surface contact, such as resulting from exposure by spills or leaks. In properly-prepared waste storage areas, undamaged paint and sealant helps to protect the structural cement. However, damaged surfaces, cracks, and relatively porous slab seams can offer a preferred migration pathway for spilled contaminates, including radionuclides. The cost of remediation of concrete structures is directly related to the amount of concrete that must be removed and subsequently disposed. A carefully implemented investigative plan can be utilized to determine how much concrete must be removed and the approximate level of volumetric radiological contamination can be used to estimate disposal costs. Normal concrete pore solution is saturated with calcium hydroxide and also contains sodium and potassium hydroxide; the pH is typically 13 to 14. Contaminants (such as uranium) that hydrolyze in alkaline media that form precipitant phases and tend to deposit at the near-surface. However, more soluble contaminants, such as Cs-137 (as Cs{sup +}) and Tc-99 (as the pertechnetate anion TcO{sub 4}{sup -}) diffuse more rapidly (and deeply) into the porous substrate. Profiling the migration of the water-soluble radionuclides into a cure (hardened) cement surface is a challenge, since water-cooled saws, borers and similar implements are often used to excise and/or slice the core. Alternately, dry mechanical fracturing for excavation of cement may introduce the possibility of material cross-contamination and uncertainty for the average sampling depth for the sample collection event, potentially yielding non-representative samples, and may preclude determination of crack formation that may have been present in the native (non-fractured) substrate. Structural concrete is comprised of cement and pozzolan paste, relatively impervious aggregate (typically stone and/or sand), and rebar (iron reinforcement). Near-surface aggregate may act as a hydrolytic barrier, causing contaminants leached into the pore water to by-pass the impervious grains, causing deeper-than expected penetration, especially if there are grain boundary cracks also present to facilitate migration. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Immobilization of Organic Liquid Radioactive Waste (LWR) in a Sulfur Composite Matrix at the BN-350 Fast Neutron Reactor Site, Kazakhstan - 18031

The immobilization treatment and final disposition of all forms of organic radioactive liquids, such as pump oil, spent solvent, tri-butyl-phosphate (TBP) and scintillation fluids, remain a significant challenge for nuclear waste generators and national regulators. The majority of nuclear nations have instituted regulations that require some form of encapsulation of treated organic liquid, notwithstanding LLW organic liquids that can be safely incinerated. In most cases cement is the designated material for encapsulation; however, cement can pose certain problems with the containment of treated organic liquids. In 2013, with funding from the U.S. Department of Energy - National Nuclear Security Administration through its Global Initiative for Proliferation Prevention Program (GIPP), a proven U.S. technology for the treatment of radioactive organic liquids was introduced at the BN-350 fast neutron reactor facility in Aktau, Kazakhstan. As the facility was undergoing full decommissioning, one hundred and sixty cubic meters of contaminated pump oil (including Cs-137, Sr-90 and U-235/238) contained in large above ground tanks had to be treated for final disposal. As a result of the research conducted over a two-year period, a new 2-step treatment process was invented by combining the U.S. solidification technology with a newly developed inorganic filler and molecular sulfur, referred to as radiation-resistant composite (RRC) to fully encapsulate the waste oil. The outcome of extensive test program indicates that the final form can reach up to 60 wt.% with a compressive strength of about 100 kg/cm{sup 2}. Preliminary conclusions indicate that RRC outperforms cement as an encapsulation form for final waste treatment which meets U.S. Nuclear Regulatory requirements for final disposal. This paper examines the preliminary experimental work that was conducted in Kazakhstan with the U.S. polymer technology and radioactive pump oil, and the subsequent secondary process of combining the solidified material into a homogeneous final form utilizing RRC. Topics covered in the paper include: - Kazakhstan's regulatory requirements for attaining an achievable waste form for acceptance, which led to the RRC invention; - Technical objectives for the application of polymer technology and RRC materials to radioactive liquid waste; - Polymer solidification with radioactive oil and the result; step one of the RRC process; - Description of RRC materials, their origin and chemical characteristics; - Process of combining the solidified polymer mass with RRC materials into a solid, homogeneous matrix; step two of the RRC process; - Experimental results including leaching data, waste loading estimates and heat process calculations to create the matrix; - Cost advantages of the RRC process over cementation; - Limitations of the RRC process; - Next steps to verify conformance of the RRC technology to the U.S. requirements. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗