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Die Hauptfunktion von Verschlussbauwerken für End- und Zwischenlager von radioaktiven Abfällen besteht in der Erhaltung der geologischen Barriere. Vor allem soll ein potenzieller Stofftransport durch eine möglichst geringe Permeabilität des Bauwerks verhindert bzw. auf vernachlässigbare Werte herabgesetzt werden. Die in-situ-Permeabilität des Verschlussbauwerks steht dabei in direktem Zusammenhang mit dessen Poren- und Makrostruktur, welche bei Bauwerken auf Basis von Beton insbesondere durch Schwind-verformungen und durch thermisch induzierte Rissbildung infolge der Reaktionswärmeentwicklung des Bindemittels gestört werden kann. Die Betone müssen daher neben einer hohen chemischen Langzeitstabilität auch eine geringe bzw. langsame Wärmeentwicklung während der Erhärtungsreaktionen aufweisen. Als hybride Zemente werden Mischungen aus Portlandzement, Betonzusatzstoffen und einem alkalischen Aktivator bezeichnet. Dabei können u. a. Alkalisulfate, Alkalicarbonate, Alkalisilicate und Alkalihydroxide als Aktivatoren zum Einsatz kommen. Aufgrund ihrer hohen chemischen Stabilität im salinaren Milieu sind Betone aus solchen Zementen potenziell besonders gut als Verfüllmaterial für End- und Zwischenlager im Steinsalz geeignet. In der vorliegenden Studie wurden daher hybride Zemente hinsichtlich ihrer Wärmeentwicklung in einem isothermen Kalorimeter sowie hinsichtlich Phasenbestand und Festigkeiten untersucht. Hybride Zementleime wurden auf Basis von Portlandklinker, Hüttensandmehl, Flugasche und Natriumsulfat hergestellt und die Zusammensetzungen systematisch variiert, um den Einfluss der Komponenten auf Wärmeentwicklung, Phasenbestand und mechanische Eigenschaften der Leime zu untersuchen; zusätzlich wurden zu Vergleichszwecken ein Zementleim auf Basis der Betonrezeptur M2 sowie eine alkalisch aktivierte Flugasche untersucht.
While calcined clays in general have been credited with a great potential to mitigate CO2 emissions related to cement production and consumption, calcined brick clays are currently understudied in this regard. In the present work, two brick clays, a low-grade kaolinitic clay, and a mixed clay composed of 50% brick clay and 50% low-grade kaolinitic clay were studied regarding transformations on calcination, and strength and durability performance as well as pore structure of mortars made with the blended cements. All calcined clays exhibited pozzolanic reactivity, with the performance of the brick clays inferior to the low-grade kaolinitic clay. However, the mixed clay performed very similar to the low-grade kaolinitic clay, which points to a viable option for optimal use of brick clays in cementitious systems. The carbonation resistance of the blended cement mortars was generally worse than that of the plain Portland cement mortar, as expected, but the former exhibited a significantly improved chloride penetration resistance. The latter improvement was due to pore structure refinement in the blended cement mortars, compared to the Portland cement mortar.
Properties of alkali-activated mortars with salt aggregate for sealing structures in evaporite rock
(2021)
Concrete structures for sealing of tunnels in the host rock are an essential part of systems for nuclear waste storage. However, concretes based on blended cements or magnesium oxychloride cements, which are commonly considered for this application, can deteriorate severely due to a significant heat of hydration and associated deformation and cracking. Alkali-activated materials (AAMs) offer a potential solution to this problem because of their low heat release during hardening. To explore their suitability for the construction of sealing structures in evaporite rock, various AAMs with salt aggregate were studied regarding fresh properties, heat release, mechanical properties and microstructure. The heat of reaction of the AAMs was up to 55% lower than that of a blended cement designed for sealing structures, indicating significant benefits for the intended application. Other relevant properties such as mechanical strength and permeability depended strongly on the mix-design of the AAMs and curing conditions.
Alkali-activated materials are ideal for the repair of concrete structures in harsh environmental conditions due to their high durability in chemically aggressive environments. However, slag-based mortars, in particular, are prone to shrinkage and associated cracks. In this respect, the application of steel fibres is one solution to reduce the formation of shrinkage induced cracks and to improve post cracking behaviour of these mortars. This study investigated the influence of two different types of steel fibres on the tensile properties of two alkali-activated mortars. Direct tensile tests and single fibre pull-outs were performed to analyse the determining failure modes both on macro and micro scale. Mechanical testing was accompanied by non-destructive testing methods such as digital image correlation and acoustic emission for a detailed analysis of the fracture process.
Two brick clays (rich in 2:1 clay minerals) and a low-grade kaolinitic clay were studied regarding their transformations during calcination and their performance in blended cement mortars. The mortars with calcined clays exhibited decreased workability (slump flow), but this effect could be mitigated by employment of a conventional superplasticizer; however, compressive strength of the hardened mortar was lowered in some cases. While the kaolinitic clay generally yielded the highest strength, the performance of a brick clay could be increased by grinding to higher fineness and by mixing it with the kaolinitic clay.
Additive manufacturing of alkali-activated materials currently attracts a lot of attention, because of the possibility to produce customized high-performance elements for a range of applications, potentially being more resource-efficient than conventionally produced parts. Here, we describe a new additive manufacturing process for alkali-activated materials that is based on selective laser-heating of lithium aluminate/microsilica slurries. The new process-material combination allows to manufacture elements with complex geometries at high building rates and high accuracy. The process is versatile and transferrable to structures of sizes differing by orders of magnitude. The mechanical strength of the obtained materials was in the range of values reported for conventional metakaolin-based geopolymers, and superior to what has been hitherto reported for alkali-activated materials produced by additive manufacturing. This mechanical performance was obtained despite the fact that the degree of reaction of the lithium aluminate and the microsilica was low, suggesting that significant reactions took place only at the surface of the microsilica particles.
Einkomponentige alkaliaktivierte Bindemittel (AAB), d. h. AAB, bei denen der Aktivator als Feststoff im Bindemittel vorliegt, weisen Vorteile hinsichtlich der praktischen Anwendung im Bauwesen gegenüber konventionellen AAB auf. Einkomponentige AAB lassen sich als Gemische aus reaktiver Silica und Natriumaluminat herstellen, wobei die Reaktionsprodukte von der eingesetzten Silica und den Verhältnissen Na2O/Al2O3/SiO2/H2O abhängen: Während Mikrosilica und ähnliche Reststoffe zu zeolithreichen Produkten führen, erhält man aus Reisschalenasche vollständig amorphe Gele (sog. «Geopolymere »). Mörtel auf Basis solcher Bindemittel entsprechen den Anforderungen von DIN 19573:2016-03 hinsichtlich des Widerstands gegen Schwefelsäureangriff (Prüfung bei pH = 1 für 70 d) und sind damit potentiell als Reparatursysteme für Abwasserinfrastruktur geeignet. Untersuchungen mittels 29Si-MAS-NMR und 1H-29Si-Kreuzpolarisations(CP)-MAS-NMR sowie REM-Aufnahmen von erhärteten und dem Schwefelsäureangriff ausgesetzten AAB zeigen, dass der hohe Säurewiderstand v. a. auf die Fällung von Silicagel an der Grenzfläche Mörtel/Säure zurückzuführen ist, wodurch der Korrosionsfortschritt in darunterliegenden Schichten verlangsamt wird.
The use of calcined clays as supplementary cementitious materials (SCMs) has been identified as a viable option to decrease the CO2 emissions related to cement production. However, while extensive data is available about kaolinitic clays in this context, other clays such as illitic clays appear to be under-studied. Therefore, in the present study, two illitic clays were compared to two low-grade kaolinitic clays in terms of transformations in the calcination temperature range 650–900 °C, and performance of the calcined clays in blended cement pastes as measured by strength evolution, heat release, hydrated phase formation and portlandite consumption. The illitic clays required a higher calcination temperature for complete dehydroxylation of their illite than what is necessary for dehydroxylation of kaolinite. These higher calcination temperatures also led to particle sintering, significantly decreasing the specific surface area of the illitic clays, particularly for the clay with the higher Fe2O3 content. Nevertheless, while the kaolinitic clays generally exhibited the best performance as SCM, the illitic clay with lower Fe2O3 content performed similar to the kaolinitic clays when calcined at optimum temperature and applied at a moderate substitution rate. These findings demonstrate that several different clays have the potential to be used as SCM and indicate possible routes to identify suitable deposits for this purpose.
Der kritische, Korrosion auslösende Chloridgehalt für die Beurteilung der Korrosions-beständigkeit von Betonstahl in Geopolymerbetonen ist von großer Bedeutung für die Dauerhaftigkeitsprognose für bewehrte Elemente aus solchen Materialien. Es sind kaum experimentelle Daten in der Fachliteratur vorhanden und die vorliegenden Werte unterscheiden sich zwischen den Studien erheblich. In diesem Projekt wurde der kritische, Korrosion auslösende Chloridgehalt für Betonstahl (BSt 500) in flugaschebasierten (Ca-armen) Geopolymermörtel für verschiedene Beaufschlagungskombinationen bestimmt: Chloridbeaufschlagung mit 1 M NaCl-Lösung; Auslaugen in entionisiertem Wasser und anschließende Chloridbeaufschlagung im 1 M NaCl-Lösung; Auslaugen in entionisiertem Wasser, Carbonatisierung in Luft bei 20 °C und natürlicher CO2 Konzentration und anschließende Chloridbeaufschlagung mit 1 M NaCl-Lösung. Für Referenz-Zwecke wurde zusätzlich der Korrosion auslösende Chloridgehalt für eine Portland-Zement Mischung bei Auslagerung in 1 M NaCl-Lösung bestimmt.
Mixing and curing of geopolymers and related alkali-activated materials without storage and handling of highly alkaline solutions possesses advantages regarding safety and economic viability. One possible approach is to produce these materials from solid silica feedstocks and solid sodium aluminate, and subsequent mixing with water. We present a comparison between geopolymers and aluminosilicate gel-zeolite composites synthesized by this route from different silica feedstocks (by-product silica from chlorosilane production, microsilica, rice husk ash) and with different SiO2/Al2O3 ratios, using results from XRD, NMR, SEM, thermal analysis, mechanical and acid resistance testing. The use of rice husk ash favors formation of a fully amorphous geopolymer with high strength. Utilization of the other silica feedstocks leads to formation of aluminosilicate gel-zeolite composites, the amount and kind of zeolites depending on the feedstock and the SiO2/Al2O3 ratio. These composites show beneficial dehydration behavior, viz. no distinct dehydration step of thermal strain, with the phase assemblage after heating to 1000°C controlled by the starting composition. Mortars produced from both, the geopolymers as well as the composites, exhibit high resistance to sulfuric acid attack, making them promising materials for the construction and the repair of industrial and sewer structures.