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Due to environmental concerns regarding the use of Portland cement as the principal binder material in concrete and mortar it is imperative to identify alternative materials that could reduce the carbon footprint of the construction industry. One alternative to address these issues is the use of alkali activated materials, in particular, when based on waste streams that currently have no or only limited industrial application. This paper reports a preliminary study into the synthesis of geopolymer mortar utilizing Brown Coal Fly Ash. The ash had a CaO content of ~39%, indicating that synthesis at ambient or low temperature may be feasible. The paper reports initial trials on the effect of curing temperature, ambient to 120 °C, on the mechanical properties of the mortars produced. The results showed that ambient cured mortar achieved a compressive strength of 6.5 MPa at 3 days. A curing temperature of 60 °C gave the optimum results with a compressive strength of almost 20 MPa and a flexural strength of 3.5 MPa obtained.
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.
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.
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.
The influence of starting materials and synthesis route on the properties and the structure of cementitious sodium aluminosilicate gels is not fully understood, partly due their amorphous nature and the fact that they often contain residual reactants, which can make the results of single-pulse NMR spectroscopy applied to these materials difficult to interpret or ambiguous. To overcome some of these limitations, 29Si{27Al} TRAPDOR NMR as well as 27Al{29Si} and 27Al{1H} REDOR NMR spectroscopy were applied to materials synthesized by the one-part alkali-activation route from three different amorphous silica starting materials, including rice husk ash. The latter led to formation of a fully amorphous sodium aluminosilicate gel (geopolymer), while the materials produced from the other silicas contained amorphous phase and crystalline zeolites. Application of the double-resonance NMR methods allowed to identify hydrous alumina gel domains in the rice husk ash-based material as well as significantly differing amounts of residual silica in the three cured materials. Four-coordinated Al existed not only in the aluminosilicate gel framework but also in a water-rich chemical environment with only a small amount of Si in proximity, likely in the alumina gel or possibly present as extra-framework Al in the aluminosilicate gel. The results demonstrate how the employment of different silica starting materials determines the phase assemblage of one-part alkali-activated materials, which in turn influences their engineering properties such as the resistance against chemically/biologically aggressive media.
Mortars for application on concrete, e.g. repair mortars or protective coatings, need to have a durable bond to the substrate. This bond is determined by the adhesion between the two materials and by the differential deformations of the mortar and the substrate. In the present contribution, the hygric deformations (shrinkage/expansion) of novel one-part alkali-activated mortars and their bond to concrete substrates are studied. Shrinkage of the mortars was studied at 50 % r.H., while expansion was studied on mortars stored over an open water surface (> 99% r.H.). The bond behaviour was studied by pull-off tests according to DIN EN 1542 and by optical microscopy.
The alkali-activated mortars exhibit hygric deformations much lower than the deformations of an established, commercial mortar for sewer maintenance that was tested as reference in parallel with the alkali-activated mortars. The bond behaviour of the alkali-activated mortars depends strongly on their mix-design and curing. Optical microscopy showed that in the
mortars with lower bond strength, cracks developed in the mortar during curing. Mortars with appropriate mix-design and curing did not exhibit cracking, and their pull-off strength (up to >3 MPa) conformed to the requirements of relevant standards.
Two hybrid alkaline cements (HAC) based on Portland clinker, ground granulated blast furnace slag (GGBFS), fly ash and sodium sulfate, as well as an alkali-activated GGBFS/fly ash blend and a Portland cement paste were exposed to a saturated saline solution for 70 days. The combined chemical attack of chloride, magnesium and sulfate ions and the associated changes of the phase assemblage of the materials were studied by X-ray diffraction, thermal analysis and spatially resolved X-ray fluorescence spectroscopy. The experimental results revealed dissolution of ettringite, C-N-A-S-H and calcite, and the formation of gypsum, Kuzel's salt and Friedel's salt; thermodynamic modeling indicated the formation of M-S-H. The resistance of the HAC against attack by the saline solution increased with Portland clinker fraction. The capacity of portlandite to maintain pH at values above 10 is found to be a major factor controlling the resistance of HAC against corrosion in the saline solution.
Portland cement is one of the principal sources of anthropomorphic CO2 emissions. It is estimated that cement production contributes up to 10% of greenhouse gas emissions and annual cement production over 4 billion tons. This has led to the development of a range of alkali activated materials (AAM), the most common precursor materials being class F fly ash and blast furnace slag. At present Class C Fly Ash is not widely utilized as an AAM due to the chemical composition and activation requirements. However, initial research on high Calcium German Class C Fly Ash suggests that the material may have potential for application as an AAM. This paper reports the development of ambient cured alkali activated mortar optimised by varying the alkali modulus and w/b ratio. The evolution of the mechanical and microstructural properties is reported over the initial 28 day period. Compressive strength in excess of 10 MPa at 7 days and 15 MPa at 28 days was achieved at ambient temperature. Similar strengths were observed for both 10% and 15% dosage but as dosage increases the optimal Alkali Modulus reduces.