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This study investigates deep learning-based backscattered electron (BSE) image segmentation as a novel approach to automatise phase quantification of cementitious materials and estimate their degree of hydration and porosity. The case study was on Portland cement paste that hydrated from 1 day to 2 years. The initial findings suggest that using arbitrary thresholds for phase segmentation, a strong correlation can be established between the results from BSE image analysis, quantitative XRD, and EDS/BSE, particularly for samples with a hydration age >28 days. The second part demonstrates the success of automated image segmentation that relies on learning the material composition from a meticulously analysed image database, which can then predict the content of numerous other images within seconds. This novel approach can turn the analysis of cementitious materials’ phase composition from a tedious process that requires specialised equipment and expertise into a routine test for quality control.

Sol-gel processing allows synthesis of low-energy glasses. In this work, binary magnesium silicate glasses with various MgO contents are synthesized using a modified sol-gel route. TGA and XRD analyses indicate that amorphous glasses with up to 50 mol% MgO can be obtained at 500°C. The reactivity of the glasses is evaluated to assess the use of the sol-gel technique in the large-scale synthesis of alternative cementitious materials. Reactivity tests show that, as MgO content increases, reactivity of glasses increases, reaches an optimum and then declines. This trend doesn’t agree with the theoretical one estimated by NBO/T value, which is generally used for the evaluation of glass reactivity. Mg²⁺ ions play a role as the network modifier when first introduced to silicate glasses. This leads to the depolymerization of the networks, causing an increase in reactivity. Then the magnesium partly behaves as a network former, bonding with oxygens to form MgOₓ polyhedron when there are insufficient primary glass-forming oxide SiO₂, resulting in the polymerization of networks, hence the decrease in reactivity.

Partial replacement and co-hydration of calcium aluminate cement (CAC) with ladle slag was investigated in this study as a pathway in valorizing the slag and reducing the economic cost of CAC. The impact of this replacement on the physical and microstructural properties were analysed using different techniques such as mechanical strength test, freeze-thaw, sulfate attack, XRD, SEM etc. Thermodynamic modelling was used to predict the phase assemblages of the blended cement using the hydration kinetics of the system. Experimental results showed the reference CAC mortar and the substituted mortar exhibited comparable strength gain at 7 and 28 days, and durability as measured by sulfate attack, abrasion, and freeze-thaw resistance. A low water-to-binder ratio (0.35) lessened the effect of conversion on the hydrates, as XRD showed metastable CAH₁₀ and C₂AH7.5 as the hydrates at 7, 28 and 60 days. This however can convert later to the thermodynamically stable phase C₃AH₆. Thermodynamic modelling suggests these two metastable phases as major binding phases, while Si-hydrogarnet and FeOOH appeared a minor trace in the binder. *Cement chemistry notation used, where C = CaO, A = Al₂O₃ and H = H₂O

With increasing interest in utilizing metallurgical slags for mineral carbonation, there is a need to find applications for carbonated slags. The scope of this study is to explore the utilization potential of carbonated steel furnace slags (SFS) as supplementary cementitious materials (SCM) to produce low-CO₂ cement-based materials. Two different types of SFS are studied with comparable amounts of major oxides but significantly different mineral phase compositions. In the first phase of the study, several parameters that affect the CO₂ uptake during mineral carbonation are considered (temperature, CO₂ pressure, particle size, and duration) for the two slags namely, basic oxygen furnace slag (BOFS) and desulfurized slag (DeSS). Among the two slags, the DeSS exhibited significantly higher degrees of carbonation than BOFS, and the higher carbonation of DeSS is attributed to the presence of Ca as Ca(OH)₂ rather than Ca–Si in BOFS. For both the slags, increase in temperature and CO₂ pressure generally led to increase in the degree of carbonation. In the second phase of the study, 30 wt% of white Portland cement (WPC) was replaced by carbonated slags (used as SCM) in the cement mixture. The cement mixture with the BOFS carbonated at 60 °C and 1 bar CO₂ pressure, as SCM, exhibited compressive strength comparable with that of WPC. Higher degrees and rates of carbonation under different conditions appears to have reduced their reactivities as SCM.

Green liquor dreg (GLD) is a side stream generated by pulp industry. Due to its complex physicochemical nature, it has been reported to be difficult material to utilize. Here, a novel approach towards utilization of moist and dry green liquor dreg as binder and filler in alkali-activated lightweight artificial aggregates was developed. Dried GLD and moist GLD were granulated with blast furnace slag (BFS) and Bioash in different mixtures using alkali activation. The effect of the GLD nature (dried and moist) on strength, microstructure and durability of the lightweight granules were determined and compared. Results show that the method used in homogenizing the moist GLD and other powders was efficient and improved the frost resistance. The reaction product identified in the granule’s includes calcium silicate hydrate, Mg–Al layered double hydroxides, and ettringite. These results demonstrate the potential of GLD as a binder and fillers in cementitious applications.

Alternative alkali activators are a growing research area in the field of alkali-activated materials (AAMs) because conventional chemical-based activators, such as sodium hydroxide and sodium silicate, have a large environmental footprint and high costs. Industrial residues are widely studied as substitutional cementitious materials in concrete and precursors in AAMs but not much as activators. In the present study, sodium rich waste from pulp mill was used as an alkali source in AAMs. Recovery boiler fly ash (RBA) is dust-like waste fraction removed from flue gases of recovery boiler by electrostatic precipitators. It consists mainly of alkalis, sulfate, and carbon while sodium sulfate is the main phase. This work utilized RBA as a sole one-part alkali activator for a precursor mixture containing 95 wt% of blast furnace slag and 5 wt% of cement, and the results were compared with two references, one without activator and the other activated with commercial sodium sulfate. The setting properties and strength gain were comparable between the RBA-activated and commercial activator-activated samples. Calorimetry data showed also similar reactivity between them, and X-ray diffractometry, thermogravimetric analysis, and scanning electron microscopy measurements revealed that the same phases were formed. The main issue was the microcracking of the paste samples when using RBA as an activator. Results confirm the earlier findings from the literature, the activator dosage did not greatly impact the properties: in this study, the initial proportion of 1% or 3% Na2O was the most suitable.

Sodium-rich green liquor dregs (GLD) are one of the main landfilled residues generated in pulp mills, and to date, no economically profitable ways to utilise GLD has been identified. In this study, GLD have been studied to be used as an alternative alkali source together with alkali-activator, sodium metasilicate (Na₂SiO₃), for blast furnace slag (BFS) mortar. Microsilica was used as an additional silica source to ensure steady Na₂O:SiO₂-ratio (0.16). In purpose to remove the remaining organic carbon and increase the suitability of GLD to be used in alkali-activated materials, it has been first thermally treated in 525 °C. The amount of GLD in the recipes varied from 0 to 45 wt%. Calorimetry measurements showed that increasing the amount of GLD reduced the hydration heat and postponed the reaction. With thermogravimetric analysis, X-ray diffractometry and scanning electron microscopy it was found that hydrated samples with more GLD contained more carbonate phases, which indicated that the reactivity of GLD was lower in comparison with that of other raw materials. Compressive and flexural strength measurements showed that increasing the amount of GLD affected the early strength gain (2 and 7 days) of the samples, but at the age of 29 days, the difference was not as high. The compressive strength of the reference sample at 29 days was 59 MPa, while the compressive strength of four sample recipes containing GLD (up to 36 wt%) was higher than 49 MPa. According to the results, green liquor dregs have potential to be used as a secondary alkali source in alkali-activated materials, but more detailed study should be conducted for the recipe in the future.

Integrating supplementary cementitious materials (SCMs) in cement-based construction materials is a key strategy for reducing environmental burdens and the greenhouse gas emissions related to cement production. Supplies of commonly applied SCMs such as fly ash and blast furnace slag are becoming limited, and therefore the search for alternative SCMs is of high significance. The present research investigates the viability of four paper mill ashes collected at different stages from the same incineration process as SCMs at different cement substitution rates (5–30 wt%). The ashes were first classified depending on their mineralogical and chemical composition, and their contribution to strength development of the prepared mortars is examined. Furthermore, the effects of the ashes on the hydration kinetics and the fresh and hardened properties of the prepared mortars were studied. The obtained results showed that a high level of SCM replacement accelerates the early hydration reactions and decreases the setting time. In addition, the incorporation of paper mill ashes increased the bound water depending on the ash type and resulted in strength development of the mortars at low replacement per- centages (5–10 wt%). This study shows that the ashes belonging to type C medium acid based on bio ash classification could be incorporated as SCMs at a maximum level of 10 wt%, while those corresponding to type C low acid could be used up to 20–30 wt%.

Characterizing and understanding the mechanisms underlying geopolymerization are critical in achieving the use of sustainable construction material, geopolymer, for widespread commercial production. Non-destructive ¹H NMR relaxometry can provide novel information about geopolymerization as it allows simultaneous detection of where the water goes and how the pore structure changes. Coupled with the development of single-sided NMR devices, NMR measurements are not limited by the specimen size and are therefore able to observe in-situ conditions of geopolymer synthesis. Here, the curing process of metakaolin-based geopolymers was monitored by ¹H relaxometry on a single-sided NMR device. The silica-to-alumina ratio (Si/Al) was found to affect reaction stages of the geopolymerization. After the dissolution of aluminosilicate precursor, the low Si/Al of 1 was found to generate three gelation/polymerization stages as well as a water-binding stage, and two gel phases appeared. When Si/Al varied in 1.5–2.5, two gelation/polymerization stages and only one gel phase was observed.

Solid-state electrolytes (SSEs) are considered as the most promising materials for enabling the safer, more efficient, and feasible solution to address the market demands for lithium-ion batteries. The current work investigates the production of inorganic SSEs from silicate minerals, which are abundant materials in natural resources (kaolinite) as well as in industrial waste-streams (amorphous silica). The synthesized materials showed high amorphous contents combined with lithium silicate phases at variable proportions, according to the molar proportions of the reacting system. The materials have been characterized with XRD, SEM/EDS, FTIR, TGA-DSC, XPS, EIS, and density measurements. The results showed that hybrid structures of amorphous and crystalline silicates can form an ordered hotchpotch morphology. The best of the hybrid SSEs presented ionic conductivity values of 1.42 × 10-4 and 1.30 × 10-4 Scm-1 for samples with total amorphous contents of 73 and 83 wt%, respectively. The connected structure between amorphous and crystalline phases in a hotchpotch structure is hypothesized to assist the hopping of the Li+ ions via combined mechanisms of segmental motion of the silicates amorphous chains with defects in the crystalline phases. The proposed approach may offer new research paths towards the low-cost scalable production of SSEs.

Sulfidic mine tailings are potential waste materials from mining and mineral processing, and they can contain a high content of sulfur and metal(loid)s, even after bioleaching. Due to the large amount of tailings waste from historical mining, it is crucial to find alternative methods for utilizing such waste rather than permanent storage in tailings impoundments. One-part alkali-activated slag mortars are promising co-binder systems for the recycling of sulfidic mine tailings thanks to their practicability, easy transportation, and user-friendly production. In this work, up to 50 wt% mine tailings were incorporated into alkali-activated blast furnace slag mortars. C-(N)-A-S-H gels were formed in all final samples with hydrotalcite zeolites. Tailings hardly participate in alkali activation, but they do have a considerable influence on physical and chemical properties. The 20 wt% tailings-containing sample showed the highest compressive strength of 91.1 MPa after 90 days of curing. The results of isothermal calorimetry indicate that incrementally increasing the percentage of tailings promotes the pre-induction reaction but hinders the slag hydration process. In addition, the results of X-ray microcomputed tomography showed higher porosity when the mortar contains more tailings; thus, the sample with 10 wt% mine tailings showed the lowest porosity. According to the European Union batch leaching test, up to 20 wt% bioleached sulfidic mine tailings can be valorized in a co-binder system while remaining below the nonhazardous waste thresholds.

This paper details the effect of fiber reinforcement on mechanical characteristics of by-products based one-part alkali activated material (AAM). Two different binder matrices were considered in this study, such as, plain slag, and ternary blended slag, to understand their efficiency in fiber reinforced system. These matrices were reinforced with 1% v/v of three different fibers (steel, glass and basalt) to improve the flexural performance of high strength mortar blends. Steel fiber reinforced one-part AAM outperforms mineral fibers in compressive strength contribution. The fracture energy of steel fiber reinforced compositions was roughly 4 times higher than that of mineral fiber reinforced materials. In addition, the flexural performance of ternary blended matrix was higher than that of slag-based composition regardless fiber types and properties. Finally, preliminary finite element modelling was considered to assess the applicability of the concrete damage plasticity constitutive model in predicting the nonlinear behavior of the developed composites. The numerical predictions proved the accuracy of the model with good agreement between experimental and numerical results.

This paper reports on the synthesis and characteristics of a novel aluminosilicate glass-based cementitious binder. We investigated the hydration kinetics, degree of reaction, and phase assemblage of the glass via XRD, DTG, ²⁷Al and ²⁹Si MAS NMR, FTIR, SEM/EDS and thermodynamic modelling. The glass exhibits hydraulic properties in which the binder developed impressive compressive strength at early age. The main hydration products are an intermixed of Na and/or Al incorporated in C–S–H gel. Hydrotalcite precipitated with slower rate and thus may generate crystallization pressure on the binder at late stage. The glass reached a high degree of hydration (ca. 73 % based on quantitative ²⁹Si NMR analysis) without using any activators or co-binding systems. Therefore, the developed glass reported herein has high potential as a new low-carbon cementitious binder since it can be synthesised from naturally occurring carbonate free silicate minerals.

Geopolymers are alumino-silicates with inborn mesoporous structures. For construction applications, the knowledge on the porous structure and fluid dynamics is important. In this work, the interconnected pore structures of metakaolin-based geopolymers and dynamics of guest molecules were studied by 129Xe nuclear magnetic resonance (NMR), by exploiting the high sensitivity of the 129Xe chemical shift to its local environment. The 129Xe NMR spectra revealed three different pore structures experienced by xenon gas in the geopolymers: the first associated with microporous zeolite-analogous cages (≤2 nm), the second with the mesopores (2–50 nm) and the third with free Xe in larger voids. The sizes of mesopores, heat of adsorption as well as pore connectivity were determined as a function of water-to-solid (w/s) ratio. The results show that the pore structures can be tailored by changing the w/s ratio, providing tunability both for potential construction, catalysis, and adsorbent applications.

The cement industry faces an increasing demand for new supplementary cementitious materials (SCMs) as alternative to slags and ashes, the sources of which are in continuous depletion. This study reports on the characteristics of synthetic aluminosilicate glasses derived from basalt composition (BGs) as new SCMs. The pozzolanic activity of the developed glasses as well as their influence on the hydration kinetics, microstructure, and mechanical properties of blended cements are reported. The obtained results show that pastes containing BGs demonstrated faster hydration rate and higher compressive strength compared to those containing commonly applied granulated blast furnace slag (GBFS). In addition, the developed glasses demonstrated higher pozzolanic activity than GBFS as demonstrated form the measured amount of portlandite and strength activity index. The developed glasses can be obtained from earth abundant carbon-free raw materials as it is similar in composition to basalt. Therefore, this novel approach has potential to provide low-carbon cementitious binders for the concrete industry.

Porous ceramics were generated by direct foaming the alkali-activated unprocessed kaolin (impure kaolin, iK) with the addition of hydrogen peroxide (H₂O₂) and calcining at a low temperature of 400 ​°C. Hydrogen peroxide, a blowing agent, decomposes producing oxygen gas bubbles forming the porous structure in the fresh alkali-activated iK paste. In the present study, three different molarity of alkali activator (5, 10, or 15 ​M NaOH) were employed. The dosage of blowing agent (H₂O₂) was varied between 0 and 2% with a constant dosage of 0.5% (wt. of binder) of surfactant. The gas bubbles in fresh-state geopolymer slurry are unstable with a tendency to coalesce. In such cases, surfactants are introduced to improve the stability of the gas-liquid interface. Two different surfactants: non-ionic and cationic ones were used to study the properties of alkali-activated porous material. Fresh properties such as viscosity, yield stress, foaming rate, and fresh density were compared between reference iK samples without surfactants and those with surfactants. The mechanical and microstructural properties of alkali-activated (AA) low-temperature porous iK ceramics were determined after calcination. Pore structures were characterized with electron microscope to understand the interaction of different parameters during fresh/hardened state and their relevance with the changes in the mechanical properties. Surfactants, irrespective of the type, highly influenced the fresh properties of the AA-iK samples, which in turn reflected on the compressive strength of the porous ceramics.

This paper focuses on the development of high-strength and eco-friendly one-part (i.e., dry-mix) alkali-activated mortar with ground granulated blast furnace slag as the main precursor. In addition to slag, phyllite dust and silica fume were used as co-binders in binary and ternary blends to improve mechanical properties. Particle packing optimization was employed for the mix proportioning to achieve a compact matrix skeleton. The results revealed that a 10% increase in mortar strength was gained after adjusting the particle packing and an additional 20% increment was observed after blending the slag with other mineral admixtures. Ternary blend with all three binders achieved a mortar compressive strength value of 145 MPa (at 28 d age), which is the highest strength reported in one-part alkali-activated materials. Additionally, ternary blends present potential economic benefits because of their ability to replace slag with lower-cost industrial side streams.

There is some ambiguity regarding the fate of Mg during the alkali activation of Mg-rich precursors within the broader field of alkali activated materials (AAMs). The present work addresses this issue by studying the reaction products in AAMs synthesized from (Na-Mg) aluminosilicate glasses. Here, instead of magnesium silicate hydrate (M-S-H) phase, Mg exclusively forms an amorphous magnesium silicate (AMS) phase. Compared to M-S-H, AMS is a more depolymerized phase, which has not previously been well documented. The formation of AMS seems to be driven by the high charge density of the Mg cation which effectively stabilizes the depolymerized silicate species. We also show that the lack of hydrotalcite-group phases is due to aluminum depletion by zeolite formation. This work highlights the need to consider the existence of the AMS phase in Mg-containing AAMs, especially in complex systems, where its identification may be difficult.

Geopolymers are emerging construction materials with lower carbon dioxide emissions compared to the conventional cementitious materials. The knowledge of the curing process and the related pore structures are important for optimizing the properties of these materials for different applications. The curing process and final pore structure are sensitive to the amount of used water, however the specifics are unclear. The curing process and pore structures of metakaolin-based geopolymers with a narrow water-to-solid (w/s) ratio (0.59–0.66) were monitored by nuclear magnetic resonance (NMR) relaxometry and cryoporometry. The 14-day curing process was investigated by monitoring the change of T₂ and T₁ relaxation times and water signal intensity. After the curing, the pore structures were characterized by 2D T₁-T₂ correlation and T₂-T₂ exchange measurements of absorbed water. The pore size distributions (PSDs) were measured with NMR cryoporometry and compared to nitrogen physisorption and mercury intrusion porosimetry (MIP) results. We found that the relaxation times decreased as the pore structure of the geopolymers matured during the curing while the dissolution and the condensation periods of the curing were distinguished by the changes in signal amplitude reflecting the proton density. After the curing, three distinct pore sizes and connectivity between pores were identified from T₁-T₂ and T₂-T₂ spectra. Their PSDs were measured, and they were found to correspond to two different pore sizes originating from the arrangement of clusters and defective pores. In the narrow w/s ratio (0.59–0.66), the curing times were the same for all samples when cured at 24 °C while the pore sizes were observed to increase as a function of the w/s ratio.

Little is known about the performance of ettringite-based binders in hydrothermal conditions. This investigation aims to gain insights into the phase evolution and corresponding mechanical performance of an ettringite-based binder considering crystallization pressure caused by late-reaction products. Additionally, the role of fiber reinforcement on the strength retention of the binder was investigated. When aged at an elevated temperature under water-saturated conditions, hard-burned MgO hydrated to form brucite. The precipitation and growth of the brucite crystals led to a crystallization pressure of approximately 200 MPa calculated using thermodynamic modelling. Damage was observed after 4 months of aging with cracks in the microstructure and eventually a failure at the macro scale. Ettringite remained stable at 60 °C due to the water-saturated conditions. Polypropylene fiber delayed crack propagation and thus reduced the damage caused by crystallization pressure. The fiber improved the flexural performance of composite attaining deflection-hardening behavior regardless of aging conditions.

This study aims to obtain insights into the retardation mechanism of citric acid in an ettringite-based binder from ladle slag and gypsum. The hydration kinetics and phase assemblage of the binder were experimentally investigated and thermodynamically modelled. Additionally, the effects of citric acid on synthetic ettringite were studied to obtain further understanding of the interaction between this organic ligand and the crystal. Experimental results reveal that citric acid works as an inhibitor of ettringite’s formation leading to the precipitation of monosulfate and gypsum; the ettringite surface blockage by citrate ligand effectively prevents precipitation of this crystal. This leads to an overestimation in the precipitation of ettringite in the thermodynamic model due to this kinetic barrier imposed by the ligand. Thermodynamic modelling suggests ettringite, monosulfate, aluminum hydroxide, and strätlingite as main hydrates in this binder, whereas an intermixed C–(A–)S–H gel was observed experimentally instead of strätlingite.

This study evaluates the effects of the manufacturing process and fiber reinforcement on low-velocity impact response of the recently developed PVA fiber-reinforced alkali-activated stone wool composites. To this end, reinforced and unreinforced specimens manufactured by hot-pressing were compared with those oven curing. The results revealed a similar impact response for the hot-pressed composite produced at 120 °C for 3 h and its counterpart cured at ambient pressure at 60 °C oven for 24 h. Furthermore, fiber reinforcement significantly improves the impact resistance of the hot-pressed composites showing about a 50% increase in peak load and a 40% reduction in penetration compared to the unreinforced materials. In view of the development of the hot-pressed composites and potential applications, accurate predictive models are of extremely importance, hence the material mechanical behavior was here simulated by adopting the concrete damage plasticity model to predict the low-velocity impact response of both unreinforced and reinforced materials and successfully verified for the scaling-up purpose.

The generation of glass wool waste and mine tailings has raised increasing concerns. This paper deals with the reuse of glass wool waste and lithium mine tailings from spodumene ore (quartz feldspar sand; QFS) in the development of building ceramic materials. The effect of glass wool particle size and sintering temperatures (750, 850 and 950 °C) were investigated. Phase composition and sintering reactions were studied using several techniques including X-ray diffraction with Rietveld refinement, differential scanning calorimetry, scanning electron microscopy, density, water absorption and mechanical tests. The results showed that glass wool acted as fluxing agent, with melting reactions observed from about 700 °C. Grinding glass wool improved its reactivity, enhancing densification and strength development at lower temperatures. The properties of the prepared building ceramics satisfied the requirement of building materials according to ASTM C62, achieving high performance values of 90 MPa and 25 MPa for compressive and flexural strength respectively. These results are of interest for the reuse of glass wool waste, QFS and similar waste streams in building ceramics.

In this investigation, ettringite-based mortars were synthesized from ladle slag (LS) and phosphogypsum (PG), promoting the concept of a circular economy. However, the reuse of naturally occurring radioactive materials (NORM), such as PG, requires radiological investigation. Also, the immobilization degree for contaminants contained in PG should be evaluated. The former was investigated using gamma spectroscopy and radon exhalation/emanation tests, while the latter was assessed using an up-flow percolation column test according to the CEN/TS 16637‐3. The produced mortars comply with current legislation on naturally occurring radionuclides (NOR) in building materials, proving that they can be safely used for building purposes. The radon emanation decreased upon increasing the Polish PG content, which was mainly determined by the microporosity. The specific surface areas were 20‐30 times lower than conventional cement, and the immobilization degree for contaminants was generally high (>90%). This investigation demonstrates high potential for PG reuse in ettringite-based mortars.

The alkali activation of mine tailings is of interest to diminish the impoundment storage of large waste stream from mining industry. However, most of the mine tailings, like phosphate mine tailings generated in Finland, are rather inert and need pre-treatment to induce the reactivity for alkali activation. In this work, mechanochemical treatment was conducted to improve the reactivity of phosphate mine tailings. The ground specimens were subjected to the crystal structural analysis of X-Ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and thermal analyses by Thermogravimetry/Differential Thermal Analysis (TG/DTA), showing the increment of amorphous content and structural degradation as a function of grinding time. The subsequent alkaline reactivity test illustrated incremental alkaline dissolution of Si, Al and K and a schematic diagram of altered phlogopite structure (sources of aluminosilicates in tailings) was also proposed. Additionally, the mineralogical composition of individual particles was carried out by mineral liberation analysis (MLA), thereby evaluating the influence of pre-treatment on the mineralogy of tailings. The results indicate profound micromorphological changes and structural cleavage of the precursor due to grinding, which strongly increase alkaline reactivity.

Concerns about the management of glass wool waste, approximately 800,000 tons of which are generated annually in Europe, are increasing. To test the feasibility of incorporating this waste into ceramic materials, this study examined the reuse of glass wool as a fluxing agent in the production of clay- and waste-based building ceramics. Commercial kaolin clay and two industrial residues, namely quartz-feldspar sand (QFS) and copper slag (CS), were selected as the precursors. Six compositions were prepared, three samples containing glass wool and three counterparts without glass wool, and then sintered at 750, 850, and 950 °C. The materials and prepared ceramics were characterized by employing x-ray diffraction (XRD), scanning electron microscopy (SEM) coupled with energy dispersive x-ray spectroscopy (EDS), differential scanning calorimetry (DSC), water absorption, apparent density, and compressive and flexural strength tests. Interestingly, the results indicated that incorporating 10 wt% of glass wool into the QFS, CS, and kaolin mixtures created ceramics with better physical, mechanical, and microstructural properties. This was ascribed to the glass wool melting reactions observed from approximately 700 °C. The QFS samples with glass wool and sintered at 950 °C achieved compressive strength values as high as 117 MPa and water absorption percentages as low as 2%. However, the fluxing effect of glass wool was less significant in the CS- and kaolin-based ceramics, likely due to differences in their chemical composition, mineralogy, and particle-size distribution. The results of this study emphasize the reuse potential of glass wool and other waste streams in building ceramics and could contribute to improving the management of glass wool waste in line with social sustainability objectives.

Alkali-activated materials (AAMs) are alternative binders that can be used instead of Portland cement in construction. One of the main drivers in their utilization is that AAMs can be designed to have lower CO2 emissions using industrial residues. The main component of AAMs is aluminosilicate precursor, which is frequently waste based. However, the sustainable profile and cost-efficiency of AAMs are greatly affected by the selection of the alkali activator. Commonly used activators include bulk chemicals, such as sodium hydroxide or silicates, which have a relatively high carbon footprint and cost that can inhibit AAM applicability for large-scale construction applications. Consequently, several locally available, but underutilized, agricultural and industrial by-products or wastes have been investigated as alternative alkali activators. Globally, millions of tons of these residues are produced annually, and currently, they are mostly landfilled. Utilization of these residues as alternative alkali activators not only solves the residues-management issue, but also has noteworthy economic and environmental benefits. Utilization and properties of these waste-based activators in AAMs are comprehensively reviewed in this manuscript. Various studies showed the formation of alkali silicates from amorphous silica residues, alkali hydroxides, carbonates, and aluminates sourced from biomass and industrial residues. The resulting binder exhibited similar reactivity to commercial activators and considerable binder strength. However, the durability, shrinkage, and workability properties were not investigated in most of the reviewed studies.

This paper deals with the synthesis and thermal stability of one-part metakaolin geopolymer composites containing high volume of spodumene tailings (Quartz Feldspar Sand; QFS) and glass wool (GW). One of the objectives of the study was to prepare materials encompassing a maximum amount of waste streams with some potential thermal stability. Several compositions were prepared with sodium metasilicate anhydrous (Na2SiO3) wt.% of 0.5, 2.5, 5, 10 and 12,5. The one-part metakaolin geopolymer composites were cured at 60 °C for 24 h and the mechanical properties were assessed at 7 days and after post-heat treatment at 500, 750, 1000, 1100 or 1200 °C. X-ray diffraction, dilatometry, scanning electron microscopy and thermogravimetry analyses were used to study the stability of the prepared geopolymer composites until 1100–1200 °C. The results showed that more than 20 MPa compressive strength could be achieved with metakaolin geopolymer composites containing only 20 wt% of metakaolin. Metakaolin-GW geopolymer composites were stable up to 500 °C. Meanwhile, their counterparts containing QFS were stable up to 1100–1200 °C; samples prepared with higher dosage of sodium (Na2SiO3 > 5 wt%) retained more than 50% of their initial strength after thermal treatment at 1100 °C. Interestingly, for dosages of Na2SiO3 ≤ 5 wt%, more than 300% increase of strength was observed after thermal treatment at 1100–1200 °C. The use of QFS limited the thermal shrinkage at mild temperatures (<1000 °C), but favoured densification and strength development at 1100–1200 °C.

Low-alumina mine tailings (MTs) have shown the possibility of being a precursor in the production of alkali-activated materials (AAMs). The effects of the addition of sub-micron MTs (10 wt%) with the average size of 400 nm to improve the performance of AAMTs with alkali activator (10, 15, 20, and 30 wt% sodium silicate) were investigated by using X-ray diffractometry (XRD), Attenuated total reflection-Fourier-transform infrared spectroscopy (ATR-FTIR), scanning electron microscopy (SEM), and nitrogen adsorption technique (BET). The mechanical properties of the materials were also analyzed. The results indicate that the addition of sub-micron MTs to AAMTs plays an important role in mineral compositions and enhances the mechanical strength performance in comparison to plain AAMTs, especially after just 7 days of aging. This result is attributed to the different microstructure between AAMTs and sub-micron MTs. BET results showed that the addition of sub-micron MTs reduces the total porosity of alkali-activated products and changes the pore structure. The pores of AAMTs were refined by the filling effects of sub-micron particles and the enhancement of the hydration process due to the nucleation effect of those sub-micron particles. This could be a significant reason for the increase in early age mechanical strength. This work introduces a novel approach to improve the performance of tailings-based alkali-activated materials using nano-sized precursors.

The main objective of this paper was to investigate the alkali activation of mine tailings (MT) after mechanochemical activation and the effect of metakaolin (MK) addition. Finnish mica-rich tailings from a phosphate mine were studied as precursors for alkali-activated materials (AAM) with a potential application as a substitute for ordinary Portland cement (OPC). The principal physical properties (water absorption, apparent porosity and unconfined compressive strength) were measured for samples containing 30% to 70% tailings. Zeolite phases such as natrolite and cancrinite were observed and the formation of C-(N)-A-S-H¹ and N-A-S-H gels was identified by XRD, DRIFT, FESEM-EDS and NMR technologies. A life cycle assessment (LCA) was conducted on specimens in comparison to OPC. This work indicated that phosphate MT can be recycled through alkali activation with lower CO₂ emission compared to all-metakaolin geopolymers and that the binder phase formed at the most promising tailings contents (60– 70%) was C-(N)-A-S-H gel.

Mining activity is inevitable in human societies, and thus, disposal of mining waste in a proper and effective way is crucial to preserving our environment. In this context, studies on the reuse potential for mine tailings in the construction sector are booming. However, utilizing tailings as binder material is complicated due to the high variation in mineralogical composition and the low reactivity of these materials. In this study, an attempt was made to understand the effect of mechanical treatment on silicate mine tailings in order to improve their properties for use as a sole precursor in alkali-activated binders. Two different silicate tailings from Finland were studied: one rich in tremolite, which is high in magnesium (HM tailings) and one rich in anorthite and epidote, which is high in aluminum (HA tailings). Interestingly, grinding activity performed at different durations affected the properties of the tailings with various intensities, including their mineralogical and physical properties and characteristics and, thus the reactivity of tailings. Tremolite does not respond to milling for longer durations, and layered anorthite was easily distorted by the mechanical disturbance. Irrespective of the type of tailings, the compressive strength of alkali-activated milled tailings increased with an increase in grinding time from 1 to 16 min. However, the percentage of compressive strength increase varied with the type of tailings and their mineralogy.

In this study, the use of desulphurization dust (DeS-dust) generated as a waste material during steel-making process, as an alternative activator to commercial sodium hydroxide in ground granulated blast furnace slag (GGBFS) alkali activation is proposed. The main objective was to decrease the environmental footprint of alkali-activated materials through the reuse of industrial residues. Microsilica was added to increase the amount of soluble silica and enhance the properties of the investigated binders. The results indicate that binders from alternative activator performed better, achieving a 28 days maximum strength of 33 MPa compared to 25 MPa for the sodium hydroxide activated slag. Microsilica addition to the optimum mixes reduces the rate of efflorescence and increases the setting time. Also, microstructural studies using scanning electron microscopy (SEM), x-ray diffraction (XRD) and thermogravimetric analysis (TGA) show both samples having comparable gel formation and structure. Life cycle impact assessment shows significant savings that can be made using alternative activators over sodium hydroxide activated slag. Through the use of this waste material as alternative activator in alkali-activated binders, an environmentally friendly, and cleaner production of alkali-activated binders can be achieved having comparable or superior performance as the reference binder activated with commercial sodium hydroxide.

The recycling of industrial side streams is of interest for a sustainable use of resources and from an environmental perspective. This paper deals with the reuse of copper slag and spodumene tailings in the development of ceramic materials for potential application in construction. Copper slag included fayalite and magnetite as crystalline phases while spodumene tailings (quartz-felspar sand, QFS) mainly consisted of albite, quartz and microcline. Kaolin (10 wt%) was added as green strength increasing agent in some compositions and the prepared formulations were sintered between 950 and 1150 °C at 50 °C intervals. The phase composition was studied by scanning electron microscopy and X-ray diffraction using Rietveld refinement. Tests such as compressive and flexural strength, water absorption, apparent density and freeze thaw cycles were used to assess the material performances. The results showed that densification and strength development were mainly due to partial melting of QFS particles at 1050–1100 °C, leading to water absorption in the range 0.5–7 %. At 1100 °C, a high-performance compressive strength of 140 MPa was achieved with the formulation made fully of recycled materials (50 wt% copper slag and 50 wt% QFS) suggesting its suitability for high strength demanding materials such as load bearing bricks; values of ultrasonic pulse velocity and compressive strength of these ceramics remained stable after 200 freeze thaw cycles, demonstrating their potential suitability as construction materials in severe weathering environments. Additionally, the leaching test proved a good encapsulation of heavy metals in these ceramics. These results are of interest for waste management and efficient use of resources.

Carbon dioxide (CO₂) emissions from industrial processes contribute largely to the greenhouse effect and climate change. One of these industries is the cement industry, which contributes around 8% of CO₂ emissions caused by mankind. Two promising and interesting ways to reduce CO₂ emission are the utilization of alternative cementitious materials and carbon capture and utilization through CO₂ mineralization. In this study, peat-wood fly ashes from fluidized bed combustion were used as a construction material for mineral carbonation. A self-hardening characteristic of this type of fly ash was utilized, and simultaneous carbonation and hydration reactions were studied. The study showed that fly ashes from the fluidized bed combustion of peat and wood could be used to capture and mineralize CO₂ during hydration reactions. At the same time, CO₂ could improve the strength of self-hardened fly ashes. One interesting future possibility is fly ash tile production at energy plants: fly ashes can be used to capture CO₂ from flue gases, thus improving the strength of produced tiles.

Mineral wools are the most widely used building insulation material worldwide. Annually, 2.5 million tonnes of mineral wool waste are generated in the EU alone, and this is a largely unutilised material that is landfilled or incinerated. However, mineral wool wastes are promising precursors for production of alkali-activated cementitious binders due to their favourable chemical and mineralogical composition and high surface area. Alkali-activation is therefore a valuable route for valorisation of large quantities of mineral wool waste. This study resolves the phase assemblage and nanostructure of reaction products formed upon alkali activation of stone wool and glass wool by sodium hydroxide and sodium silicate solutions with X-ray diffraction, electron microscopy and solid state nuclear magnetic resonance spectroscopy experiments probing ²⁷Al and ²⁹Si. The stone wool-based alkali-activated binder comprises an amorphous sodium- and aluminium-substituted calcium silicate hydrate (C-(N-)A-S-H) gel, an amorphous sodium aluminosilicate hydrate (N-A-S-H) gel and small amounts of the layered double hydroxide phase quintinite and zeolite F. The glass wool-based alkali-activated binder comprises an amorphous Ca- and Al-substituted sodium silicate (N-(C-)(A-)S-H) gel. Gel chemical composition and reaction kinetics of alkali-activated mineral wools are shown to be dependent on the activating solution chemistry, with reaction rate and extent promoted by inclusion of a source of soluble Si in the reaction mixture. This work provides the most advanced description of the chemistry and structure of alkali-activated mineral wools to date, yielding new insight that is essential in developing valorisation pathways for mineral wools by alkali activation and providing significant impetus for development of sustainable construction materials.

Cementitious composite that has short molding time and high mechanical performance is favorable in pre-cast concrete industry. In this context, this study reports the use of hot-pressing technique to fabricate PVA fiber reinforced composites using alkali-activated stone wool (a waste from building insulation). Eight different mixtures were developed by varying the pressing time and temperature in comparison to the conventional oven-cured alkali-activated material. The mechanical performance of all compositions was evaluated under bending and compressive loadings. Life cycle assessment was used to investigate the greenhouse gas emission and embodied energy of the developed composites. The results reveal that PVA fibers greatly enhanced the mechanical performance of all reinforced mixtures with deflection hardening behavior and improvement in compressive strength. The hot-pressing technique lowered CO₂ emission and saved energy. Finally, a multi-criteria ranking method suggests hot-pressed PVA fiber reinforced cementitious composite, manufactured at 120 °C for 2 h, is the best composition attaining balance among energy spent, mechanical properties, and CO₂ footprint.

The synergistic combination of different nanomaterials for improved performance in environmental applications such as the removal of aqueous micropollutants has attracted increasing interest in recent years. This study demonstrates a novel sequential adsorption–aggregation concept that harnesses tubular halloysite nanotubes (HNTs) and flexible cellulose nanofibrils (CNFs) for the removal of a small, anionic dye molecule, chrome azurol S, from water. Hollow HNTs were first allowed to interact with the aqueous dye solution, after which the dye-loaded colloidal nanotubes were aggregated and separated from the water phase with cationized CNFs. The combination of 25 mg CNFs with 1 g HNTs at pH 7 resulted in efficient removal of dye (80%) and turbidity (~100%) and the removal of dye was further promoted in more acidic conditions (within the pH range of 6–8.5) because of the attractive electrostatic interactions. Cationic CNFs not only enabled the separation of dye-loaded clay particles from the water phase through a rapid aggregation but also participated in dye removal through adsorption (~20%). In comparison with nano-sized HNTs, the dye removal performance of micro-sized and chemically similar kaolin was poor (43%). Given the good availability of both HNTs and CNFs and the low consumption of the more expensive component (i.e., CNFs) in the process, the concept is straightforward, readily applicable, environmentally benign, and potentially cost-effective.

Fluidized bed combustion fly ash (FBCFA), notably different from regular (coal) fly ash, is a promising industrial side stream to be used as a supplementary cementitious material (SCM). Peat and wood are important sources of biomass for energy production in Nordic countries and generate formidable amounts of un-used ash yearly. Two FBCFAs from the co-combustion of peat and wood, fly ash from coal combustion, and limestone filler were used to replace 10 wt%, 20 wt%, and 40 wt% of cement in mortar specimens. The compressive strength, porosity, water absorption, water vapor permeability, and drying shrinkage of the mortars were measured and compared. It was found that in almost all properties FBCFAs outperformed un-reactive limestone filler. Compared to coal fly ash, FBCFAs produced mortars with comparable compressive strength although with higher porosity, water absorption, and water vapor permeability.

Ladle slag (LS) is a byproduct from the steel industry that is usually reactive on its own and hydrates towards cementitious phases when mixed with water. However, these reaction products are often metastable, leading to micro-structural changes between 7 and 30 days after mixing. To address this issue, in this experimental investigation, a new binder was designed where LS was mixed with gypsum in order to deliver an ettringite-based binder (LSG). The experimental results revealed that the dominant crystalline phase of LSG was ettringite, which remained stable with no conversion at later stages. For better understanding of the ettringite-based binder, mortar characterization, mechanical properties, and durability of LSG were investigated. LSG showed good mechanical properties and excellent freeze-thaw resistance after 300 cycles, which is comparable to other calcium sulfoaluminate cements. Therefore, as a result, the byproduct-based ettringite binder synthesized herein could offer a solution to steelmaking byproducts with a low-CO2 binder, which could be used in a wide range of applications in the construction industry.

Use of mine tailings as an aluminosilicate precursor in alkali activation is becoming an interesting alternative to manage the high-volume of waste generated from mining industries. However, very few tailings have so far been studied for their mineralogical properties and alkali activation potential. This study aims at understanding the ability of mine tailings from phosphate, kaolinite and lithium mines for their efficient participation in alkali activation. Biotite, muscovite, kaolinite, albite, and quartz were found to be the major minerals present in them. The impact of variation in mineralogy on silica and alumina solubility of these tailings was analyzed. The solubility was found to be high in impure kaolinite compared to the other two. Effectiveness of thermal treatment (750 °C and 900 °C) on improving the reactivity of these tailings in alkaline condition was also investigated. It was observed from the results that the effect of thermal treatment on the crystalline structure and solubility of an aluminosilicate material mainly depends on the mineral structure of the material, as well as the treatment temperature. Interestingly, thermal treatment reduced the solubility of lithium tailings with albite and quartz mineral. Effort has been made to relate the strength attained by alkali activation of mine tailings to their solubility values. However, despite of the higher solubility offered by impure kaolinite, phosphate tailings gives the maximum strength improvement by 62%. This can be due to the presence of calcium compounds in phosphate tailings that resulted in additional hydration products.

Soapstone is a soft, magnesium-rich mineral widely used in the production of carved objects and architectural elements, for instance. The processing of soapstone causes the formation of significant amounts of waste powder, which is largely landfilled at the moment. The aim of the present study is to evaluate the suitability of soapstone waste as the main binder for the alkali-activation process using sodium silicate and hydroxide solutions as activators. The results demonstrate that soapstone alone reacts to some extent (compressive strength of 13 MPa at 28 day age), but mechanical properties are improved significantly after replacing 20% of soapstone by metakaolin (compressive strength of 31 MPa at 28 d age). The obtained mechanical properties are closely similar to those of virgin soapstone. Durability properties of the developed alkali-activated binders were similar or better than typical Portland cement-based binders in terms of high temperature, acid, and freeze-thaw resistance, and sorptivity. The material costs alkali-activated soapstone mortar were estimated as approximately 70 €/t. Thus, the results enable utilizing currently underexploited soapstone waste in a sustainable and economically interesting way.

Aiming to utilize phosphogypsum (PG) as a construction material, this study investigated the potential use of PG as a calcium sulfate source for the production of an ettringite-based binder (LSG). Six compositions with different percentages and PG’s of different origin were hydrated with ladle slag (LS) to form LSG. The hydration, mineralogy and compressive strength of all mixtures were investigated and compared with a reference LSG made of pure synthetic gypsum. The minor impurities in PG, the different particle size distribution as well as the mineralogy induced distinguishable effects on the heat of hydration, phase assemblage and morphology. The results showed that the use of side-stream PG instead of pure gypsum results in superior properties with a 60% increase in compressive strength. This investigation shows high potential to produce a completely by-product-based LSG by combining different sources of industrial side-streams with minimal chemical and energy use.