The growing incineration of municipal solid waste results in hazardous byproducts, particularly municipal solid waste incineration (MSWI) fly ash and air pollution control (APC) residues. The high toxicity of these residues limits their potential for recycling, leading to their direct disposal in landfills. This landfilling poses a significant environmental risk and presents a major challenge in countries with limited availability of land, such as the Netherlands. In this study, the physicochemical properties of Dutch MSWI fly ash and APC residues were evaluated, including, for the first time, an assessment of trace metal concentrations. High concentrations of heavy metals such as Zn, Pb, Cu, and Cd were identified in most MSWI fly ash and APC residues, along with notable concentrations of trace metals like Bi, suggesting new opportunities for resource recovery. The most hazardous residues were characterized by high contents of chloride, sulfate, alkali oxides, or carbonates, along with low calcium content in their chemical composition. These findings provide valuable insights for the targeted treatment and potential recycling of hazardous MSWI fly ash and APC residues currently being landfilled in the Netherlands.

Cementitious materials can achieve desirable strength development and reduced cracking potential under moist or immersed conditions. However, in this work, we found that alkali-activated slag (AAS) pastes can crack underwater, with a higher silicate modulus showing more pronounced cracking. Chemically, the C-(N-)A-S-H gel in the paste with a higher silicate modulus showed a higher Na/Si ratio and a higher leaching loss of Na, which led to more significant structural changes and gel deterioration underwater. This triggered the propagation of cracks initially present in the material. Physically, the paste with a higher silicate modulus featured a denser microstructure, lower water permeability and higher pore pressure, which resulted in a steeper gradient of pore pressure in the matrix. Consequently, the concentration of tensile stress was simulated at the centre and the corner of the cross-section of the sample. As this simulated concentrated stress exceeded the flexural strength of AAS pastes, significant fractures at the centre and spalling at the corner occurred, consistent with the experimental observation. This work not only elucidated the cracking mechanisms of AAS materials underwater but also provided new insights into mixture designs for these materials under high-humidity conditions.

Alkali-Activated Concrete (AAC) is considered as a promising alternative to conventional Portland Cement Concrete (PCC) due to its potential to reduce environmental impacts. However, its application in practical engineering is limited by, among others, insufficient understanding of the long-term structural behaviour of reinforced and prestressed AAC elements. To address this, a series of experiments were conducted on composite girders to investigate the long-term flexural behaviour. The composite girder is formed by a prefabricated prestressed AAC inverted-T girder with cast-in-situ ACC topping concrete. The midspan deflection of two composite girders, subjected to self-weight and additional sustained loading, were measured over a 9-month period. Subsequently, flexural tests under four-point bending configuration were performed at the age of 9 months and the reference age of 28 days. The results showed that the specimens tested at 9 months exhibited reduced initial stiffness, decreased cracking load and larger crack widths in the precast prestressed girder compared to those tested at 28 days. The reduction in stiffness likely stems from decreased elastic modulus and structural cracking. Meanwhile, the lower cracking load arises from prestress losses caused by ongoing (restrained) shrinkage and creep, consistent with AAC material test observations. Larger crack widths observed in the precast girder may result from a degradation of bond between AAC and prestressing strands over time. The distinct failure patterns of the 9-month specimens (anchorage failure for sample subjected to self-weight only and flexural failure for sample exposed to additional sustained load), highlighted the role of creep on bond behaviour between prestressing strands and AAC, particularly as a function of varying stress levels at the level of strands. Finally, analytical models were applied to evaluate the prestress loss and flexural behaviour of the specimens. The effective prestressing force and cracking loads at both testing ages were overestimated when the effects of (partially) restrained deformations between precast and cast-in-situ AAC were neglected. More accurate analytical predictions were achieved when these long-term effects and the level of restraint in the composite girder were considered.

This research investigated the use of wood biomass fly ash (WBFA) as a key component in developing low-carbon cementitious materials. WBFA was first subjected to water pretreatment and grinding to remove metallic aluminum and free lime, reducing expansion and cracking risks. Characterization of WBFA showed its high calcium and alkali-bearing phases but limited aluminosilicates. Dissolution test showed WBFA had strong alkalinity, suggesting its role as an activator for aluminosilicate-bearing minerals. A novel cement- and chemical-free binary binder was developed using 50 % treated WBFA and 50 % blast furnace slag (BFS). Paste with a water-to-binder ratio of 0.4 achieved 40 MPa compressive strength at 60 days. The use of superplasticizer significantly improved flowability, allowing the water-to-binder ratio to be reduced to 0.25, which resulted in compressive strength up to 58 MPa at 60 days. Calcium aluminate silicate hydrates (C-A-S-H) gels and ettringite were identified as the main reaction products in the pastes.

Existing research on the mechanisms affecting the strength of cementitious materials primarily focuses on the composition and properties of cement hydration products, often overlooking the interactions between different products. This study presents a systematic experimental and theoretical investigation into the mechanical properties of cementitious materials, emphasizing the interactions between crystal and gel products driven by crystallization pressure. A new mechanism based on crystallization pressure is proposed to explain the impact of the interactions between hydration products on the strengths of cementitious materials. Experiments were conducted by immersing specimens in solutions with tailored ion concentrations (including water, isopropyl alcohol, ethanol, and solutions of calcium hydroxide and calcium acetate) to vary the crystallization pressure. The flexural and compressive strengths of these specimens were then tested. An analytical model was developed and validated against the experimental data. Both experimental and calculated results demonstrate a negative correlation between crystallization pressure and strength. Specimens subjected to crystallization pressures of 101.7 MPa and 147.8 MPa showed reductions in flexural strength of 19.34 % and 30.65 %, respectively, and decreases in compressive strength of 10.00 % and 14.41 %, compared to control specimens with zero crystallization pressure. These results suggest that ion concentrations in the pore solution alter the crystallization pressure, which in turn affects the interactions between crystal and gel products and strength of cementitious materials. This study provides insights into the mechanisms of strength degradation due to moisture in porous materials.

This study focuses on the numerical modeling of the reaction and microstructure development of a one-part granite-based geopolymer, which is often used for carbon capture and storage (CCS) applications. This work extends the capabilities of GeoMicro3D to model one-part geopolymers containing different precursors and activators (solid and in solution). The model considers the particle size distribution of different solids and the real shape of particles to prepare the initial simulation domain. Further, the dissolution rates of different solids estimated from the experiments were used to model the dissolution of different elements in the pore solution. Subsequently, the model utilizes classical nucleation probability modeling coupled with thermodynamic modeling to estimate the precipitation of products in the microstructure. Experiments were performed to study the pore solution, reaction degree, and amount of products in the microstructure, which were further compared with the simulation results to check the rationality of the model.

Efflorescence is a significant aesthetic and structural issue for alkali-activated materials (AAMs). This study addressed this issue at the aggregate level for the first time. The results indicated that substituting sand with aluminosilicate-based lightweight fine aggregate (LWFA) by 20 % or 50 % in volume reduced the efflorescence of alkali-activated slag (AAS) mortars by 14.6 % or 43 %, respectively. The mitigation mechanisms of LWFA were proposed in terms of gels, pore solution and microstructure. Specifically, the pozzolanic reaction of LWFA provided gels with additional Si and Al, which contributed to binding Na⁺ in the pore solution, thereby reducing the available Na for efflorescence formation. Combined with its internal curing effect, LWFA densified the surrounding pastes, which hindered the transport of ions and water, thus limiting the formation of efflorescence products. Furthermore, the incorporation of LWFA enhanced the flexural strength of mortars without significantly compromising compressive strength.

Compared with blast furnace slag (BFS), the less reactive MSWI bottom ash (MBA) plays a minor role in alkali-activated blends. This research optimized the use of MBA as a precursor by enhancing its contribution to strength and microstructure development. The proposed strategy combines pre-treatment with pre-activation processes, enabling MBA to react before BFS addition. The NaOH-based pre-treatment led to the oxidation of metallic aluminum and the partial dissolution of the amorphous phase in MBA. The subsequent pre-activation resulted in the generation of C-A-S-H gel, which promoted later-stage gel formation in the paste. The reacted bottom ash particles exhibited distinct features in alkali-activated pastes. Compared with 100 % slag-based system, blending slag with MBA accelerated the slag reaction at late ages and facilitated the formation of a more polymerized C-(N-)A-S-H gel. The compressive strength results indicate that MBA is a promising alternative to Class F coal fly ash in BFS-based alkali-activated blends.

While ensuring the long-term integrity of wellbore sealants is critical for the success of geological carbon storage (GCS), the chemical degradation of conventional materials under CO₂-rich conditions remains a major challenge. This study investigates the carbonation behavior of a one-part granite-based geopolymer, integrating a novel pore-scale simulation framework with experimental validation. A new model, ReacSan, is developed to simulate CO₂ transport and carbonation reactions within the evolving microstructure of the geopolymer under GCS-relevant conditions. The framework incorporates CO₂ dissolution using the Redlich–Kwong equation of state, gel dissolution via transition state theory, ion transport using the Lattice Boltzmann Method, and chemical reactions through thermodynamic modeling. The model was validated through experiments exposing equivalent geopolymer samples to CO₂ under in-situ conditions. The experimentally observed rapid carbonation, leading to a decrease in pore fluid pH and the precipitation of CaCO₃ matched the numerical simulations well, demonstrating the ability of the novel ReacSan framework to capture both temporal and spatial variations in the microstructure and carbonation mechanisms of alkali-activated materials (AAMs) exposed to supercritical CO₂. Based on the demonstrated validity of the model, the model is capable of providing detailed predictions of carbonation progression of AAMs or any other sealants over longer time- and length-scales required to ensure long-term GCS integrity.

This study presents an extended numerical approach based on GeoMicro3D to simulate the reaction kinetics and three-dimensional (3D) microstructure evolution of alkali-activated fly ash (AAFA). Dissolution experiments were conducted under varying NaOH concentrations and temperatures to formulate predictive rate functions for Si and Al release. These experimentally derived kinetic functions, alongside a thermodynamic dataset for N-(C-)A-S-H gels, were incorporated into the GeoMicro3D model to capture the chemical reactions and 3D microstructure evolution of AAFA. The model well captured reaction degree of fly ash, formation of solid products, evolution of pore solution compositions, and porosity over time. Notably, it is the first to predict the time-dependent spatial distribution of phases within the 3D AAFA microstructure by integrating kinetic and microstructural modeling. Dual validation using both dissolution data and microstructural metrics demonstrates the model's reliability and robustness. This integrated framework provides new insights into the coupled chemical–microstructural evolution of alkali-activated materials.

Alkali and alkali earth metal ions are normally present in the gels of alkali-activated materials as well as blended PC-based materials. Previous studies have revealed that the leaching of these cations can trigger the change in gel structure and even the gel decomposition. However, the dissolution of cations was rarely known and the underlying mechanisms remained unclear. To address this issue, five calcium-(sodium, potassium-)aluminum-silicate hydrates (C-(N,K-)A-S-H gels) with different Ca/Si ratios (0.8–1.2) and Al/Si ratios (0.1–0.3) were synthesized to investigate the leaching behaviour of Ca, Na and K. For the first time, the dissolution free energies of Ca, Na and K in C-(N,K-)A-S-H gels were calculated using molecular dynamics simulations with the metadynamics method. Experimental results showed that Na showed the highest leaching ratio, followed by K and Ca, attributed to the lowest dissolution free energy of Na. The gel with a higher Ca/Si ratio or a lower Al/Si ratio showed higher charge positivity on the surface, resulting in reduced leaching of the three cations. Additionally, the presence of K was found to promote the dissolution of Na in gels.

The equivalent conductivities of two aqueous silicate species, [SiO(OH)3]− and [SiO2(OH)2]2−, are fundamental to understanding many physico-chemical phenomena of silicate materials in electrolyte solutions. These phenomena include diffusion, adsorption, and phase transformations. But significant inconsistencies have been presented in published equivalent conductivities of the two silicate aqueous ions. Also, little work has so far been undertaken to discuss how aspects, such as temperature and solution composition, may influence electrolytic conductivity of silicate aqueous solutions. This work presents the equivalent conductivities of the two silicate species, measured with electrochemical impedance spectroscopy (EIS) from 277.85 K to 308.45 K. A conductivity model for mixed electrolytes of high alkaline was first established. This model was then verified with the electrolyte conductivities of NaOH-H2O solutions and NaOH-Na2CO3-H2O solutions. Next, the equivalent conductivities of [SiO(OH)3]− and [SiO2(OH)2]2−, were calculated by solving the overdetermined equation groups for different temperatures, based on electrolyte conductivities of NaOH-Na2SiO3-H2O solutions. The accuracy of both calculations and measurements are examined in depth from various viewpoints. This work presents essential inputs for quantitatively understanding multiple physico-chemical properties of silicate materials in electrolyte solutions.

Wood biomass fly ash (WBFA) has emerged as one of the most dominant by-products in the biomass energy sector. Circulating WBFA for construction practice can mitigate the secondary pollution caused by improper ash management, and provide a new material source to compensate for the scarcity of raw materials in the construction industry. This paper reviewed the current research progress on recycling WBFA in cementitious materials. The physicochemical properties of WBFA were summarized based on the literature. Further, the implementations of WBFA for the development of cementitious materials were categorized into three binder systems: clinker, blended cement, and alkali-activated materials (AAMs). Owing to the large variation in chemical compositions of WBFA and strict requirements in clinkering parameters, employing WBFA in blended cement and AAMs seems to be more promising. A new classification approach for WBFA was proposed to divide WBFA into two categories. This helps to provide simple guidance for ash recycling in construction practice. Finally, the current research gaps in WBFA valorization in cementitious materials were summarized, outlining the research for further exploration.

To properly control the reaction kinetics and fresh properties evolution in conventional alkali-activated materials (AAMs), a conceptual design of two-stream AAMs has been proposed in this study. This is achieved by dividing the solid and liquid components in AAMs, including blast furnace slag (BFS) and electric arc furnace slag (EFS) precursors, as well as aqueous sodium hydroxide and silicate activators into two separate streams A and B, where a very limited reactivity is expected in individual streams to ensure sufficient workability retention. Moreover, a final-stage intermixing is required to combine individual stream mixtures and trigger the major activation reaction. Fresh and hardened properties of combined mixtures were checked at different stages. The microstructure and reaction products were investigated to understand the strength development. Low dynamic rheological parameters and good workability retention have been detected in all individual stream mixtures, accompanied by limited exothermic heat flows after the initial dissolution confirmed by calorimetry tests. Further, Portland cement (PC) is partially blended into stream A to alter the early stiffening process in combined mixtures and meet various setting demands after intermixing. However, this might lead to a reduction in mechanical properties, associated with the formation of porous microstructures and an increase in the Ca/Si ratio in reaction products. Eventually, the conceptual design is validated in different scenarios including self-compacting and 3D-printing concrete applications.

As the main waste product of iron and steel industry, steel slag possesses considerable cementitious activity, making it a promising alternative to cement in Cement Stabilized Macadam (CSM). However, CSM was inevitably exposed to groundwater and rainwater when served as the pavement base course, leading to concerns over poor early strength and potential pollutant leakage, which are the main factors that may hinder the widespread utilization of steel slag in CSM base. To address these issues, this study investigated the feasibility of using steel slag powder to produce CSM. Steel Slag Powder-Cement Stabilized Macadam (SSCSM) samples were prepared and the hydration products, microstructure, mechanical properties, water damage resistance and heavy metal ions leaching behavior were investigated. The results show that the nucleation effect of steel slag powder accelerates the early hydration, but the C-S-H produced by hydration is not sufficient to form a stable hydration product network, so the microstructure of SSCSM is looser than that of CSM. The addition of steel slag powder improved the shrinkage performance of SSCSM, and the mechanical properties and heavy metal ion leaching concentration of SSCSM meet the engineering application requirements when the steel slag powder replacement level does not exceed 30 %. It was also found that the addition of steel slag powder promoted the development of pores in SSCSM samples after dry-wet cycles, resulting in the reduction of water damage resistance. Compared with conventional CSM, the use of SSCSM can not only reduce 4 % of raw material cost and 23.5 % of equivalent CO₂ emission, but also mitigate the heavy metal ions leaching risk associated with steel slag, making it an effective and sustainable solution for steel slag recycling.

While alkali-activated slag (AAS) has emerged as a promising alternative binder in construction engineering, a consensus on the optimal curing condition for this material has not been reached yet. It is well known that AAS can harden at ambient temperatures, but the influence of humidity on its properties remains poorly understood. Herein, we considered five curing conditions with different relative humidities (RH), including ambient/dry condition (RH=55 %), sealed condition (RH=80–95 %), fog condition (RH>95 %), water immersion condition (RH=100 %), and saturated limewater immersion condition (RH=100 %). Various properties have been examined, including flexural and compressive strengths, elastic modulus, shrinkage, pore structure, carbonation resistance, and freeze-thaw resistance of AAS mortars (AASM). Two types of activators, sodium hydroxide and sodium silicate (modulus at 1) solutions were used. The experimental results indicate that drying at early ages is detrimental to almost all the properties investigated. Sealed curing can deliver desirable mechanical properties and durability, but considerable shrinkage. Fog and water curings are highly effective at mitigating early shrinkage in AASM, but the problem of leaching adversely affects its long-term properties. Generally, limewater curing offers limited benefits compared to other high-humidity curing methods.

Carbonation of alkali-activated slag (AAS) materials has been primarily concerned in atmospheres with gaseous CO₂. This study, by contrast, highlights that AAS pastes would also be carbonated under tap water immersion. Calcite is the main CO₂-bear phase in both sodium hydroxide- and sodium silicate-activated AAS pastes, and the paste pre-cured for a longer curing period shows more severe carbonation. Additionally, calcium carbonate can densify the deteriorated microstructure of sodium hydroxide-activated paste caused by long-term leaching. The indentation modulus of pastes subjected to tap water immersion is higher than those under deionized water immersion. The uptake of CO₃^2- by hydrotalcite (Ht) and gels is also detected, resulting in the formation of Ht-CO₃ and decalcification of gels. Due to the synergistic effect of leaching and carbonation, a characteristic layered distribution of pastes close to the exposure front is observed, comprising the carbonated layer, transitional (carbonated + leached) layer, and leached layer, progressing from the outermost to the inner regions. Eventually, the kinetics of underwater carbonation, as well as the discrepancy between dry and underwater carbonation, is revealed.

Municipal solid waste incineration (MSWI) bottom ash, due to its high mineral content, presents great potential as supplementary cementitious material (SCM). Weathering, also known as aging, is a treatment process commonly employed in waste management to minimize the risk of heavy metal leaching from MSWI bottom ash. Using weathered MSWI bottom ash to produce blended cement pastes is considered as a high-value-added and sustainable waste disposal solution. However, a critical challenge arises from the metallic aluminum (Al) in weathered MSWI bottom ash, which is known to induce detrimental effects such as volume expansion and strength loss of blended cement pastes. While most metallic Al in weathered MSWI bottom ash can be removed with eddy current separators in metal recovery plants, the residual metallic Al, owing to its small particle size, cannot be removed with the same technique. This study is dedicated to addressing this issue. An in-depth analysis was conducted on residual metallic Al embedded in weathered MSWI bottom ash particles, aiming to guide the removal of this metal. This analysis revealed that mechanical removal was the most suitable method for extracting metallic Al. The specific processes and mechanisms underlying this method were elucidated. After reducing metallic Al content in weathered MSWI bottom ash by 77 %, a significant improvement in the quality of blended cement pastes was observed. This work contributes to the broader adoption of mechanical treatments for removing residual metallic Al from weathered MSWI bottom ash and facilitates the application of treated ash as SCM.

Given the crucial role of carbonation in the hardening of lime-based binders, accurate measurements of carbonation depths are essential for analysing both carbonation kinetics and carbon sequestration capabilities. This study employed both the conventional phenolphthalein spray method and the profile-based method to determine carbonation depths in four types of binders. Unlike the distinct carbonation front observed in cementitious materials, lime-based binders displayed a transition zone between fully carbonated and uncarbonated areas. Meanwhile, the remaining portlandite content in some specimens did not necessarily increase with depth, and typical Liesegang patterns were observed. Compared to phenolphthalein spray method, profile-based methods provide more quantitative evidence for further analyses, but inevitable slice interval can also lead to errors in carbonation depth estimation. Therefore, developing a more precise and convenient method remains essential for a deeper understanding of the carbonation behaviour in lime-based binders.

Efflorescence presents not only as a cosmetic concern but also as a structural issue, which impacts the performance of alkali-activated materials (AAMs). In this study, the mechanisms of efflorescence of alkali-activated slag (AAS) pastes are investigated. First, the efflorescence of AAS pastes with different alkali dosages (3 %, 5 % and 7 %), activator types (sodium hydroxide (NH) and sodium silicate (NS)), exposure atmospheres (ambient, N₂ and 0.2 vol% CO₂), and relative humidities (40 %, 60 % and 80 %) was observed. Subsequently, leaching tests were performed and the impacts of efflorescence on AAS pastes at different heights were studied. It was found that a lower relative humidity facilitated more rapid and severe efflorescence. The positioning of efflorescence products was dependent on the porosity of the matrix. Compared to NH pastes, NS pastes subjected to semi-contact water conditions were more vulnerable to cracking problems, which turned out to be exacerbated by the formation of efflorescence products. A new method to quantify efflorescence was developed and it corresponded well with both efflorescence observations and leaching experiments. Furthermore, a competitive reaction between Ca and Na in the presence of carbonate ions was identified. CaCO₃, a representative product of natural carbonation, was rarely found in the regions where efflorescence products (sodium carbonate) formed. Regarding compressive strength, NS pastes were more adversely affected by efflorescence than NH pastes.