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Die Zementindustrie erzeugt etwa 6-7% der globalen CO2-Emissionen und steht damit als Industriezweig vor dem Hintergrund einer anvisierten Klimaneutralität vor gewaltigen Herausforderungen. Der Prozess der Klinkerherstellung wurde über die vergangenen Jahrzehnte bereits kontinuierlich optimiert. Seit 1990 ist es der deutschen Zementindustrie gelungen, die spezifischen CO2-Emissionen der Zementproduktion u. a. durch den Einsatz alternativer, nicht fossiler Brennstoffe und durch Absenkung des Klinkergehalts im Zement um 20 % zu senken. Weitere konventionelle Minderungsstrategien versprechen jedoch nur noch wenig zusätzliche Reduktion. Im Falle des Portlandklinkers besteht die Schwierigkeit darin, dass zwei Drittel der CO2-Emissionen rohstoffbedingt durch die Entsäuerung des Kalksteins (CaCO3) anfallen, die durch die beschriebenen Maßnahmen nicht weiter abgesenkt werden können. Vielmehr wird es erforderlich sein, noch zu entwickelnde oder zu optimierende Technologien anzuwenden und ggf. alle relevanten Ebenen wie Produktion, Weiterverarbeitung und Anwendung von Zement und Beton neu zu denken. Neben technologischen Ansätzen zur CO2-Abscheidung mit nachfolgender langfristiger Speicherung (Carbon Capture and Storage – CCS) oder Verwertung (Carbon Capture and Utilisation – CCU) werden auch alternative Rohstoffe für die Zementproduktion und alternative Bindemittel in Betracht zu ziehen sein.
This study aims at investigating the use of coal fly ash-based alkali activated mortars as passive fire protection system for steel structures. These systems are used to slow down the temperature rise of the steel substrate in case of fire. In addition, the protective system should guarantee the ability to prevent and/or mitigate steel corrosion phenomena. The behavior of a light-weight mortar was compared to that of a normal-weight mortar. Density and porosity were measured to better characterize the physical properties of the mortars. The degree of protection in case of fire was assessed by performing medium-scale fire tests. Acoustic emission measurements were conducted to analyze cracking phenomena during the high temperature exposure. The corrosion process was evaluated using an electrochemical approach in order to monitor the durability of the developed material. Preliminary results show that a 20 mm-thick layer of light-weight mortar is able to protect the steel substrate from reaching the critical temperature of 500 °C for 38 minutes in case of cellulosic fire. In addition, alkali activated mortars provide protection for carbon steel in presence of aggressive environment (i.e. presence of chlorides). The corrosion resistance is strictly related to the physical properties of the developed mortars.
Alkali-activated fly ashes have been proposed for various applications where resistance against high temperatures is required, yet several details regarding the response of these materials to heat-exposure need to be clarified. In the present study, heat-induced cracking in fly ash-based alkali-activated pastes and lightweight mortars was analyzed by in-situ acoustic emission (AE) detection during complete heating-cooling cycles (up to ∼1100 °C), augmented by thermogravimetry and ex-situ SEM and XRD analyses. The applicability of the lightweight mortars as passive fire protection coatings was assessed by recording temperature-time curves of mortar-coated steel plates. Cracking during heating was limited and associated exclusively with the dehydration of the materials in the temperature range ∼90–360 °C. However, samples heated to temperatures above ∼600 °C exhibited intense cracking on cooling. This was attributed to differential deformations caused by local sintering and partial melting at the glass transition temperature, and subsequent quenching on cooling.
The present study aims to investigate the use of geopolymer mortars as passive fire protection system for steel structures. Coal fly ashes were used as aluminosilicate source and perlite was employed as aggregate to obtain a lightweight system. In addition, a geopolymer mortar containing quartz aggregate was produced for comparison. The geopolymer mortars were applied on stainless steel plates and exposed to both, cellulosic and hydrocarbon standard fire curves, according to ISO 834-1 and EN 1363-2, respectively. Acoustic emission measurements were conducted to analyze cracking phenomena during the high temperature exposure. The resulting temperature-time curves showed that the investigated system is effective in retarding the temperature rise of the steel plates. When the cellulosic fire curve was applied, a 20 mm [0.79 in.] thick layer of lightweight geopolymer mortar protected the steel substrate from reaching the critical temperature of 500 °C [932 °F] for at least 30 minutes, avoiding the rapid decrease of its mechanical properties and thus representing an important safety measure against accidental fires. No spalling phenomena on heating were detected; however, significant cracking was observed on cooling.
While alkali-activated binders offer certain advantages over traditional Portland cement binders, particu¬larly in terms of resistance against chemical attacks and potentially environmental footprint, their degra¬dation mechanisms remain incompletely understood at present, specifically carbonation. Thus, this study investigates the impact of natural and accelerated carbonation (1% and 4% CO2) on three different compositions of alkali-activated concretes: 100% calcined clay (C100) binder, 100% ground blast furnace slag (S100) binder, and a 40% calcined clay and 60% blast furnace slag blend (C40S60). C100 concretes exhibit faster carbonation kinetics, with five times greater natural carbonation depths than S100. This difference diminishes under accelerated carbonation, showing a 1.5 times difference for 1% CO2 and complete carbonation for 4% CO2 at 90 days. The results thus confirm that accelerated carbonation testing of low-Ca alkali-activated concretes yields results that are not representative of natural carbonation. The C40S60 sample demonstrates a carbonation profile similar to a CEM I concrete, i.e., a high carbonation resistance. Microstructure analysis indicates the formation of three polymorphs of calcium carbonate for S100 (calcite, vaterite, and aragonite), with a higher CO2 concentration favouring aragonite over vaterite. C100 exhibits no calcium carbonates; instead, sodium carbonates form, including trona for 4% CO2 and natrite for both accelerated tests. C40S60 shows calcium and sodium carbonates, although to a lesser extent, containing predominantly calcite and minor signals of natrite. Suitable compositions, like C40S60, prove as effective during natural or accelerated carbonation tests as conventional Portland cement concrete.
Future lunar exploration will be based on in-situ resource utilization (ISRU) techniques. The most abundant raw material on the Moon is lunar regolith, which, however, is very scarce on Earth, making the study of simulants a necessity. The objective of this study is to characterize and investigate the sintering behavior of EAC-1A lunar regolith simulant. The characterization of the simulant included the determination of the phase assemblage, characteristic temperatures determination and water content analysis. The results are discussed in the context of sintering experiments of EAC-1A simulant, which showed that the material can be sintered to a relative density close to 90%, but only within a very narrow range of temperatures (20–30 °C). Sintering experiments were performed for sieved and unsieved, as well as for dried and non-dried specimens of EAC-1A. In addition, an analysis of the densification and mechanical properties of the sintered specimens was done. The sintering experiments at different temperatures showed that the finest fraction of sieved simulant can reach a higher maximum sintering temperature, and consequently a higher densification and biaxial strength. The non-dried powder exhibited higher densification and biaxial strength after sintering compared to the dried specimen. This difference was explained with a higher green density of the non-dried powder during pressing, rather than due to an actual influence on the sintering mechanism. Nevertheless, drying the powder prior to sintering is important to avoid the overestimation of the strength of specimens to be fabricated on the Moon.
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 geopolymer-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 geopolymer-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 compo¬sites, exhibit high resistance to sulfuric acid attack, making them promising materials for the construction and the repair of industrial and sewer structures.
One-part geopolymers (OPGs) are a sort of alkali-activated materials (AAMs) which production avoids the use of highly-alkaline activator-solutions and contributes to a better acceptance of alternative mineral binders in terms of safety-related and economic aspects. In the present contribution OPGs were synthesized by blending silica sources (two industrial silicas and two biogenic silicas) with sodium aluminate and only water must be added to initiate the hardening, i.e. mixing is performed in the same way as for conventional Portland cements. The OPGs were characterized by XRD, and SEM and the degrees of reaction of the silicas were determined by a chemical dissolution method.
The industrial silicas led to the formation of geopolymer-zeolite composites, that contained, besides geopolymeric gel, crystalline tectosilicates (e.g. zeolite A and hydrosodalite) and depending on the starting composition also unreacted silica. The biogenic silicas provided a higher reactivity and avoided the formation of crystallite by-products. The differences in the microstructures caused differences in the mechanical strength of the specimens.
The treatment of the OPG composites at moderate elevated temperatures revealed promising behavior on thermal dehydration in terms of shrinkage and residual strength up to 700 °C. Above 700 °C sintering and partial melting occurred, and new phase formation commenced. After exposure to 1000 °C the specimens appeared virtually amorphous or formed stuffed silica structures of nepheline- or carnegieite-type type.
The investigations of the OPG based mortars on their resistance against sulfuric acid in accordance with DIN 19573 (Appendix A) revealed very high residual strengths up to 78 % after treatment with H2SO4 (pH 1) for 70d. A mechanism of dissolution of the primary aluminosilicate reaction products of the pastes and the precipitation of a silica gel that protects the remaining aluminosilicates and decelerates further corrosion was found to be the main reason for the good performance under acidic conditions. The addition of CaO-containing feedstocks enhanced hardening, but at a certain content the resistance against sulfuric acid decreased, due to the formation of gypsum on exposure to sulfate.
In addition, the mortars exhibited excellent shrinkage behavior as well as good bond to concrete substrates with pull-off strength up to > 3 MPa. The workability of the fresh mortars provided very good manual applicability; automatic applications such as sprayed and spun mortars will require further optimization regarding rheological properties. In summary, the studied OPG are promising materials for the construction and the repair of concrete structures, such as sewers, that are affected by biogenic sulfuric acid corrosion.
Intumescent coatings for fire protection offer advantages over (non-intumescent) cementitious coatings and boards regarding speed of construction, architectural aesthetics, sometimes costs, and other features. However, conventional organic intumescent coatings as well as soluble silicate (waterglass) coatings form foams with low mechanical stability, and the latter coatings generally suffer from low resistance against humidity. Therefore, the search for novel intumescent coatings for more demanding conditions (e.g., abrasive environments) is a necessity in the context of steadily increasing requirements of society and industry.
In this contribution, we present results on intumescent aluminosilicate coatings for fire protection that form foams with significantly increased mechanical strength. Two base formulations, a metakaolin/silica-based mix, adapted from Krivenko et al., and a silica/corundum-based mix, developed at Curtin University, as well as formulations modified with additives (Al(OH)3, Mg(OH)2, B2O3, Na2B4O7), were applied to steel plates (75 mm × 75 mm) and exposed to simulated fire conditions (fire curve according to ISO 834-1:1999). Temperature-time curves were recorded to assess the degree at which the coatings insulated the substrate. In addition, XRD, TG, oscillatory rheometry, and SEM were employed to characterise the coatings.
The coatings were observed to partly expand during hardening due to H2 formation. When the hardened coatings were exposed to elevated temperatures they intumesced as expected, with the degree and nature of expansion dependent on the formulation. Oscillatory rheometry provided insights into the intumescent processes in an apparently brittle material. It revealed that the hardened aluminosilicate coatings became viscous (loss factor > 1) at 75–225 °C, in the temperature range of major water release, as opposed to a “standard” metakaolin-based geopolymer, which continued to behave as a solid. This explains the intumes¬cent behavior of the coatings, i.e. further expansion and foam formation. Microstructural analysis confirmed pore expansion and coalescence; XRD showed that the phases formed after heating (max. temperature ~840 °C) were of ceramic-type.
The fire protection (defined here as the time for the steel substrate to reach the critical temperature of 500 °C) depended mainly on the thick¬ness of the fully expanded coating, i.e. after intumescence. An alumino¬silicate coating free of additives with an original thickness of 12 mm was able to protect the steel for >30 min. The addition of 10 % anhydrous borax (Na2B4O7) caused a significant improvement, such that an original coating thickness of only 6 mm was sufficient to protect the steel for ~30 min. This was caused by the formation of sodium metaborate dihydrate (NaB(OH)4) in the coating that led to a significantly extended dehydration plateau in the temperature-time curve at ~100 °C during the fire exposure.
Materials with a high acid resistance are required in different important infrastructures. Examples include repair systems for sewer structures, where biogenic sulfuric acid corrosion is the major degradation mechanism. Low-calcium alkali-activated materials (AAMs) have been repeatedly observed to exhibit high acid resistance. However, the reasons for the high acid resistance of these materials were not fully under¬stood until recently, and the use of highly alkaline activator solutions to produce AAMs appears to hamper their commercial uptake. These issues have been tackled by characterising one-part AAMs and studying their alteration when exposed to sulfuric acid.
One-part AAMs were synthesized by mixing blends of solid silica and sodium aluminate with water, and subsequent curing at 60–80 °C. Acid resistance testing was performed according to DIN 19573, i.e. exposure to sulfuric acid at pH = 1 for 70 days. Characterisation of the cured and the acid-exposed materials was done by XRD, ATR-FTIR, SEM as well as 29Si, 27Al and 1H MAS NMR spectroscopy, including cross-polarisation and double-resonance methods.
Materials synthesized from industrial silicas were gel-zeolite composites, containing a substantial amount of unreacted ‘excess’ silica, while materials synthesized from rice husk ash were fully amorphous, containing ‘excess’ hydrous alumina. The sulfuric acid resistance of mortars based on these binders conformed to the requirements of DIN 19573 for sewer repair applications. The high acid resistance was caused by precipitation of silica gel at the mortar–solution interface, inhibiting further degradation. The presence of alumina gel may inhibit bacterial activity, potentially further improving performance in sewer environments.
The phase assemblage of silica/sodium aluminate-based one-part AAMs can be adjusted via choice of the silica starting material. Properly designed materials exhibit excellent acid resistance, caused by precipi¬tation of silica gel which protects subjacent regions, and they may also inhibit bacterial activity.