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Eingeladener Vortrag
- nein (19)
Ground Granulated Blast-Furnace Slag (GGBFS), a by-product of the iron-making process, has gained significant attention as a supplementary cementitious material and has become increasingly popular in recent years due to its remarkable properties. GGBFS can significantly reduce the environmental impact of cement production when it comes to building concrete structures. GGBFS can either be blended with ordinary Portland cement (OPC) (up to a 90% replacement), or it can be used in the production of alkali-activated materials (AAMs). However, a comprehensive understanding of the pore solution composition is necessary for understanding various aspects of cementitious materials and their durability, including corrosion behavior, passivation of steel, and resistance to deteriorative processes. In the present work, the pore solutions of seven different GGBFS-containing cements (alkali-activated slag, alkali-activated slag/fly ash blends, a hybrid alkaline cement, CEM III/C, and CEM III/B) were extracted and analysed by inductively coupled plasma-optical emission spectroscopy, ion chromatography, pH, redox potential, and conductivity measurements. For comparison, a Portland cement pore solution was analysed similarly. The Concentrations of reduced sulfur were noteworthy in all GGBFS-containing cements, particularly in alkali-activated cements, where concentrations were notably higher compared to standard cements. The redox potentials of the pore solutions were primarily dictated by the concentrations of reduced sulfur, although other factors may contribute. Additionally, sulfur species in the pore solutions had an impact on pH, electrical conductivity, and other properties pertinent to the corrosion of reinforcements.
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.
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.
Chloride binding by the hydrate phases of cementitious materials influences the rate of chloride ingress into these materials and, thus, the time at which chloride reaches the steel reinforcement in concrete structures. A particularly important role in this context is played by layered double hydroxides (LDHs), including AFm phases. Chloride binding isotherms of individual LDH/AFm phases would be required as input for computational models of chloride ingress, but such isotherms are only available for a few AFm phases, and in addition the available data are partly conflicting.
The present study, conducted in the context of RILEM TC 283-CAM ‘Chloride transport in alkali-activated materials’, significantly extends the available database by determining the chloride binding isotherms of LDH/AFm phases (monosulfate, strätlingite, hydrotalcite, and meixnerite), and of alkali-activated slags (AAS) produced with four different activators (Na2SiO3, Na2O∙1.87SiO2, Na2CO3, and Na2SO4), in NaOH/NaCl solutions at various liquid/solid ratios. Selected solids after chloride binding were analysed by X-ray diffraction, and thermodynamic modelling was applied to simulate the phase changes occurring during chloride binding by the AFm phases.
The chloride binding isotherms of LDH/AFm phases depended strongly on the liquid/solid ratio during the experiments, resolving apparent contradictions of the previously available data. The dependency on liquid/solid ratio must be attributed to kinetic restrictions, which are, however, currently poorly understood. Chloride binding by AAS pastes was generally higher than for Portland cement pastes and was only moderately influenced by the employed activator. A steep increase of the chloride binding by AAS occurred at free chloride concentrations above approx. 1.0 M, which is possibly related to chloride binding by the C-(N-)A-S-H gel in the AAS.
The current understanding of the carbonation of alkali-activated concretes is ham-pered inter alia by the wide range of binder chemistries used. To overcome some of the limitations of individual studies and to identify general correlations between their mix design parameters and carbonation resistance, the RILEM TC 281-CCC working group 6 compiled carbonation data for alkali-activated concretes and mortars from the literature. For comparison purposes, data for blended Portland cement-based concretes with a high percentage of SCMs (≥ 66 % of the binder) were also included in the database. A preliminary analysis of the database indicates that w/CaO ratio and w/b ratio exert an influence on the carbonation resistance of alkali-activated concretes but, contrary to what has been reported for concretes based on (blended) Portland cements, these are not good indicators of their carbonation resistance when considered individually. A better indicator of the carbonation resistance of alkali-activated concretes under conditions approxi-mating natural carbonation appears to be their w/(CaO + Na2O + K2O) ratio. Furthermore, the analysis points to significant shortcomings of tests at elevated CO2 concentrations for low-Ca alkali-activated concretes, indicating that even at a concentration of 1 % CO2, the outcomes may lead to inaccurate predictions of the carbonation coefficient under natural exposure conditions.
The RILEM TC 281–CCC "Carbonation of concrete with supplementary cementitious materials" is studying the effect of supplementary cementitious materials (SCMs) on natural and accelerated carbonation of blended cements. In this context a large database with carbonation depths over time has been set-up with currently 910 concrete and mortar mixes, which have been tested at different curing conditions. The collected data includes information on chemical composition and physical properties of the raw materials, on mix-design, compressive strength, curing and carbonation testing conditions. Data for a large variety of binders (with up to 94 % SCMs) and mix designs (with w/b ratios ranging from 0.26 to 0.75) were collected from the literature and unpublished material testing projects. Natural carbonation was recorded for several years in many cases, and indoor as well as outdoor results are included. However, in this contribution only lab conditions are considered. Carbonation kinetics are investigated considering the binder composition and mix design. Furthermore, the accuracy of accelerated carbonation testing is evaluated. As described in literature, the w/CaOreactive-ratio is a decisive factor for carbonation resistance but curing and exposure conditions influence the results as well. Even with identical test conditions, the scatter is very large.
Alkalisch aktivierte Bindemittel (AAB) und Betone können herkömmliche Zemente beziehungsweise Betone potentiell in vielen Anwendungen ersetzen und dadurch den CO2-Fußabdruck der Bauindustrie wesentlich verkleinern. Zur Untersuchung der Stahlkorrosion in bewehrten („armierten“) Betonbauteilen werden elektrochemische Methoden wie Messungen des Freien Korrosionspotentials, des Polarisationswiderstands oder von Stromdichte-Potential-Kurven eingesetzt. Diese Methoden und die etablierten Grenzwerte zur Detektion von Korrosion sind für die Anwendung bei herkömmlichen Zementen beziehungsweise Betonen entwickelt und erprobt worden. Neue Forschungsergebnisse demonstrieren, dass Unterschiede zwischen den Porenlösungszusammensetzungen von herkömmlichen Zementen und bestimmten AAB sowie anderen schlackehaltigen Zementen erhebliche Unterschiede bei den Ergebnissen der elektrochemischen Messungen bewirken und damit zur fehlerhaften Detektion von Stahlkorrosion führen können. Ursache hierfür sind vor allem reduzierte Schwefelspezies in den Porenlösungen von AAB und anderen schlackehaltigen Zementen.
The safe storage of radioactive material in nuclear waste repositories is a major task of our societies. The sealing function of such repositories is depending on the ability of the applied construction materials to form and maintain a geotechnical barrier with the surrounding rock. Corrosion of the construction material can lead to leakage of radioactive compounds and must therefore be avoided or minimized. Since concretes based on conventional Portland cement have not been found suitable in this context, alternative binders must be evaluated.
One such class of binders are hybrid cements, which are blends of low fractions of Portland cement or Portland clinker and high fractions of supplementary cementitious materials, such as blast furnace slag and fly ash, activated by an alkali salt. Besides a low heat of hydration and a sufficient early compressive strength [1], chemical similarities with ancient Roman concrete suggest an excellent durability in saline environments [2], which makes these cements potentially suitable for applications in nuclear waste repositories in evaporite rock, such as the Morsleben repository in Germany.
In the present study, two previously designed and characterized [3] hybrid cements, an alkali-activated slag/fly ash blend, and an OPC paste were studied regarding their resistance against corrosion in an aggressive saline solution. The saline solution was designed by the Gesellschaft für Anlagen- und Reaktorsicherheit (GRS) [Association for Facility and Reactor Safety] as a reference representing a solution forming as the result of contact of surface water with evaporite rock. The cement pastes were exposed to the saline solution up to 70 days and characterized by X-ray diffraction, thermogravimetric analysis and spatially resolved X-ray fluorescence spectroscopy. In addition, thermodynamic modelling was performed to simulate the alterations of the phase assemblage with increasing exposure to the saline solution and, thus, provide indications on the long-term durability of the cement pastes.
The experimental results revealed a correlation between the Portland clinker content of the cements and the resistance of the cement pastes against attack by the saline solution. This outcome was related to the formation of portlandite when sufficient clinker was available, which maintained the pore solution pH at ~12.5, and thus prevented the dissolution of cementitious phases. Once portlandite was consumed, C-N-A-S-H and ettringite dissolved and released calcium, aluminium, and hydroxide ions in the solution, maintaining the pH at ~10. In this pH range, the formation Cl-AFm phases was observed. At lower pH values, i.e., extended exposure durations, gypsum was the major corrosion product. The pH-dependent dissolution and formation of phases lead to pronounced zonation in the exposed cement pastes. Thermodynamic modelling indicated that the dissolved silicon from C-N-A-S-H reacts with magnesium ions in the saline solution to form M-S-H, and that long-term exposure eventually leads to a material rich in amorphous silica and brucite.
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.
The current ability to predict the carbonation resistance of alkali-activated materials (AAMs) is incomplete, partly because of widely varying AAM chemistries and variable testing conditions. To identify general correlations between mix design parameters and the carbonation rate of AAMs, RILEM TC 281-CCC Working Group 6 compiled and analysed carbonation data for alkali-activated concretes and mortars from the literature. For comparison purposes, data for blended Portland cement-based concretes with a high percentage of SCMs (≥66% of the binder) were also included in the database. The results show that the water/CaO ratio is not a reliable indicator of the carbonation rate of AAMs. A better indicator of the carbonation rate of AAMs under conditions approximating natural carbonation is their water/(CaO + MgOeq + Na2Oeq + K2Oeq) ratio, where the index ‘eq’ indicates an equivalent amount based on molar masses. This finding can be explained by the CO2 binding capacity of alkaline-earth and alkali metal ions; the obtained correlation also indicates an influence of the space-filling capability of the binding phases of AAMs, as for conventional cements. However, this ratio can serve only as an approximate indicator of carbonation resistance, as other parameters also affect the carbonation resistance of alkali-activated concretes. In addition, the analysis of the dataset revealed peculiarities of accelerated tests using elevated CO2 concentrations for low-Ca AAMs, indicating that even at the relatively modest concentration of 1% CO2, accelerated testing may lead to inaccurate predictions of their carbonation resistance under natural exposure conditions.