Woody biomass fly ash (WBFA) is the main by-product of woody biomass energy production. However, its use in cementitious materials remains limited due to its low intrinsic reactivity, largely associated with the scarcity of aluminosilicate phases. At the same time, the high alkalinity and sulphur content in WBFA make it a promising component for formulating cement-free binders without additional chemical activators, when combined with highly reactive precursors. This study investigates the reaction mechanisms and microstructural evolution of binders based on WBFA and ground granulated blast furnace slag (BFS), with the aim of elucidating their synergistic interactions and optimizing performance. Binary pastes with varying WBFA/BFS ratios mixed with water were prepared and characterized by isothermal calorimetry, pore solution analysis, XRD, FTIR, TGA, SEM-EDS, and MIP. The results show that, although increasing WBFA content initially delayed hydration by limiting the dissolution of reactive species, it markedly enhances long-term reactivity and strength through sustained release of alkali and sulphate. The main hydration products are C-(A)-S-H gels, ettringite, Friedel's salt, and hydrotalcite, with their amount and assemblage strongly governed by the WBFA/BFS ratio. Reaction kinetics analysis and thermodynamic modelling confirm the dual role of WBFA as both a reactive precursor and internal alkali/sulphate activator. Among the formulations studied, the mixture with a WBFA/BFS ratio of 50:50 exhibited the best overall performance, achieving the highest compressive strength and lowest porosity. These findings clarify the reaction mechanisms in WBFA-BFS binary pastes, providing practical guidance for designing WBFA-based, cement-free binders for sustainable construction applications.

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.

Previously, the lack of a thermodynamic database for N-(C-)A-S-H gel limited the application of thermodynamic modeling to alkali-activated fly ash (AAFA). This study pioneers thermodynamic modeling of AAFA using a recently developed thermodynamic dataset for N-(C-)A-S-H gel. The reaction products, pore solutions and reaction kinetics of AAFA pastes were experimentally determined. Based on the reaction kinetics, the composition of the solid phases and the pore solution of AAFA were modeled over time. The results showed that the simulated compositions of the solid reaction products and pore solution match closely with the experimental results, especially for the sodium hydroxide-activated system. Moreover, modeling results point out the potential presence of minor reaction products (e.g., C-(N-)A-S-H gel, microcrystalline ferrihydrite, Mg-containing phases) undetectable by experimental techniques. The study also demonstrated that thermodynamic modeling accurately captured the amount of bound water in reaction products, highlighting its robustness in both qualitative and quantitative analysis.

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.

In our former paper, based on a published 3D reactive transport model at microscale with the capability of simulating the chemical reactions involved in ASR, the location of expansive ASR gel related to the reactivity of aggregate, temperature, aggregate porosity and silica content in aggregate, is clarified. Based on the simulation results, in this paper, the cracking process at mesoscale in concrete induced by ASR in the early stage is investigated. The results show that the cracking process can be divided into four stages and three cracking routes are generalized with the behind chemical exposed environments specified. The cracking routes are found to be comparable with the experimental observed routes. For the first time, the cracking patterns induced by ASR in concrete at mesoscale is linked with the chemical reactions at microscale, which is the first step towards building a complete computational tool to predict ASR as realistic as possible.

Prediction of alkali silica reaction is still difficult due to the lack of a comprehensive understanding of its chemical fundamentals. In-site experimentally revealing the fundamentals is not realistic as ASR shows over several years or even decades and is affected by many factors. In this paper, by utilizing a 3D reactive-transport simulation model at microscale, we have numerically explored the fundamentals of ASR in the early stage under the influence of reactive silica fraction, alkali concentration, silica disorder degree and aggregate porosity. Based on the simulation results, the chemical sequences of ASR, the initial location of ASR products, the mechanism behind and the role of calcium under the influence of the above factors are elaborated. Furthermore, a comprehensive mechanism to explain the pessimum reactive aggregate content is derived. The results of this paper give some insights about ASR in the early stage such as the initial expansion locations.

A 3D reactive transport model at microscale is proposed for simulating the chemical reaction process of alkali silica reaction (ASR) thermodynamically and kinetically including the dissolution of reactive silica, the nucleation and growth of ASR products and the dissolution of calcium hydroxide (CH) and calcium silicate hydrate (C-S-H) as a buffer of Ca²⁺ and OH⁻ to ASR. The implementation methodologies are firstly explained. Sensitivity analyses are done to calibrate some important parameters. The model is then applied to investigate the influence of the silica microstructural disorder degree on ASR. The simulation results show that the model is able to simulate successfully two typical patterns of the expansion sites location depending on the silica reactivity (inside the aggregate or in the aggregate-cement paste zone) found in field concrete and laboratory samples. A possible mechanism is provided based on the quantitative data captured by the model. The model can be extended to a multiscale ASR model for physic-chemical simulation to bridge the gap between the fundamental chemical mechanisms and the physical response of concrete.

Portland cement is the most produced material in the world. The hydration process of cement consists of a group of complex chemical reactions. In order to investigate the mechanism of cement hydration, it is vital to study the hydration of each phase separately. An integrated model is proposed in this paper to simulate the dissolution of alite under different hydrodynamic conditions at microscale, coupling Kinetic Monte Carlo model (KMC), Lattice Boltzmann method (LBM) and diffusion boundary layer (DBL). The dissolution of alite is initialised with KMC. Two Multiple-relaxation-time (MRT) LB models are used to simulate the fluid flow and transport of ions, respectively. For solid-liquid interface, DBL is adapted to calculate the concentration gradient and dissolution flux. The model is validated with experiment from literature. The simulation results show good agreements with the results published in the literature.

The microstructure of alkali-reactive aggregates, especially the spatial distribution of the pore and reactive silica phase, plays a significant role in the process of the alkali silica reaction (ASR) in concrete, as it determines not only the reaction front of ASR but also the localization of the produced expansive product from where the cracking begins. However, the microstructure of the aggregate was either simplified or neglected in the current ASR simulation models. Due to the various particle sizes and heterogeneous distribution of the reactive silica in the aggregate, it is difficult to obtain a representative microstructure at a desired voxel size by using non-destructive computed tomography (CT) or focused ion beam milling combined with scanning electron microscopy (FIB-SEM). In order to fill this gap, this paper proposed a model that simulates the microstructures of the alkali-reactive aggregate based on 2D images. Five representative 3D microstructures with different pore and quartz fractions were simulated from SEM images. The simulated fraction, scattering density, as well as the autocorrelation function (ACF) of pore and quartz agreed well with the original ones. A mm concrete cube with irregular coarse aggregates was then simulated with the aggregate assembled by the five representative microstructures. The average pore (at microscale m) and quartz fractions of the cube matched well with the X-ray diffraction (XRD) and Mercury intrusion porosimetry (MIP) results. The simulated microstructures can be used as a basis for simulation of the chemical reaction of ASR at a microscale.