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.

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.

In this paper, 871 data were collected from literature and trained by the 4 representative machine learning methods, in order to build a robust compressive strength predictive model for slag and fly ash based alkali activated concretes. The optimum models of each machine learning method were verified by 4 validation metrics and further compared with an empirical formula and experimental results. Besides, a literature study was carried out to investigate the connection between compressive strength and other mechanical characteristics. As a result, the gradient boosting regression trees model and several predictive formulas were eventually proposed for the prediction of the mechanical behavior including compressive strength, elastic modulus, splitting tensile strength, flexural strength, and Poisson's ratio of BFS/FA-AACs. The importance index of each parameter on the strength of BFS/FA-AACs was elaborated as well.

Cementitious materials exposed to marine and saline environments are commonly threatened by a combined attack of sulfate and chloride ions. This study developed a numerical framework to investigate two combined coupling mechanisms of 1) coupled solid-liquid chemical reactions for competitive chloride-sulfate attack and 2) electrostatic multi-ion coupling effect on reactive-transport mechanisms. Various chemical reactions including sulfate attack with anhydrous calcium aluminates, secondary precipitation of expansive minerals, competitive binding, and calcium leaching have been quantified. The electrostatic potential caused by multi-ions coupling was solved according to constitutive electrochemical laws. After model validation, the chemical coupling mechanisms for solid-liquid reactions during competitive chloride-sulfate binding were investigated. On this foundation, the influence of electrostatic multi-ionic coupling effects on ionic transport and its interaction with chemical coupling were disclosed. It was found that neglecting multi-ions coupling effect would result in an underestimated chemical coupling strength in competitive chloride-sulfate binding.

Alkali-activated material (AAM) is developed as a green alternative binder to replace Portland cement (PC) in the construction field. However, the large-scale application with AAM concrete is limited so far, with the insufficient knowledge of rheological behavior being a major obstruct. Thixotropy of concrete is of great interest, which can be helpful to predict various early-age performances. The current study dedicates to evaluating the thixotropy of alkali-activated slag (AAS) concrete mixtures with different silicate and water content in activator solutions. In specific, the silicate modulus (Ms) and water to binder (w/b) ratio have been varied. The thixotropic index calculated by the initial and equilibrium shear stress from the stress growth test, as well as the breakdown area obtained by applying different shear speeds were used to evaluate the thixotropy of AAM concrete. Results indicate a good correlation between different approaches. It was found that an increase in Ms led to more pronounced thixotropic behaviors in AAS concrete due to the rapid nucleation and accumulation of early hydration products, resulting in significant increases in peak torque values and slight reductions of torque at equilibrium. Besides, the concrete thixotropy gradually declined by applying a higher w/b ratio.

This study aims to interpret the early-stage rheology of alkali-activated slag (AAS) paste from microstructure perspectives. The microstructures visualized by cryogenic scanning electron microscopy (cryo-SEM) revealed the essential distinction between hydroxide and silicate-activated slag pastes. The hydroxide-based mixture showed typical suspension features, where slag particles were dispersed in the hydroxide activators. In the hydroxide media, even at very early ages (5 min), the solid grains were attached to each other through rigid connections of reaction products, which resulted in high yield stress. As for the silicate-based mixtures, an emulsion phase has been observed between slag particles, which consists of discontinuous water droplets and continuous silicate gels. Fine emulsions with smaller water droplets were observed as the silicate modulus of activators increased, which dispersed the slag particles but on the other hand improved the viscosity of the paste. With increasing water to binder ratio, both yield stress and viscosity of AAS pastes significantly reduced.

Alkali-activated materials (AAM) are known to be environmentally friendly alternatives to cement-based materials because they can potentially reduce greenhouse gas emissions and reutilize industrial by-products/wastes. To study the factors influencing the strength of slag based alkali-activated materials (BFS-AAM), fly ash based alkali-activated materials (FA-AAM), slag, and fly ash-based alkali-activated materials (BFS/FA-AAM), and clarifying their reaction mechanisms, this paper reviews current knowledge about the mechanical properties and the reaction mechanisms of BFS-AAM, FA-AAM, and BFS/FA-AAM. The precursor requirements and the strength control factors are summarized. The control factors for the strength of BFS/FA-AAM are the BFS/binder ratio, the Na₂O/binder ratio, the SiO₂/Na₂O ratio, and the w/binder ratio. Ion concentrations, determined by these control factors, play a decisive role in the development of strength. Generally, the strength is proportional to the BFS/FA ratio. The optimal values of the Na₂O/binder ratio of BFS-AAM and FA-AAM are between 5.5% and 8% and between 7 and 10%, respectively. The optimal values of the SiO₂/Na₂O ratio of BFS-AAM and FA-AAM are between 0.85 and 1.4 and between 0.6 and 1, respectively. Increasing the w/binder ratio will only benefit workability but will affect the strength negatively. A w/binder ratio of around 0.4 may strike a balance between strength and workability.

The production of cement and concrete contributes significantly to global greenhouse gas emissions. Alkali‐activated concretes (AACs) are a family of existing alternative construction materials that could reduce the current environmental impact of Portland cement (PC) production and utilisation. Successful applications of AACs can be found in Europe and the former USSR since the 1950s and more recently in Australia, China and North America, proving their potential as construction materials. However, their utilisation is limited presently by the lack of normative and construction guidelines. Raw materials’ non‐uniform global availability and variable intrinsic properties, coupled with the lack of specific testing methods, raise questions regarding reproducibility and reliability. The mechanical and chemical behaviour of AACs has been investigated extensively over the past decades, strengthening its potential as a sustainable substitute for traditional PC‐based concrete. Although a wide amount of studies demonstrated that AACs could meet and even exceed the performance requirements provided by European design standards, a classification of these broad spectra of materials, as well as new analytical models linking the chemistry of the system components to the mechanical behaviour of the material, still need further development. This report gives an overview of the potential of alkali‐activated systems technology, focusing on the limitations and challenges still hindering their standardisation and wider application in the construction field.

The present study explores the possibility of replacing blast furnace slag (BFS) with coal fly ash (FA) to produce alkali-activated material (AAM) concrete with hybrid precursors. With an increased FA replacement ratio, the reaction kinetics, fresh and hardened properties of AAM mixtures have been investigated. The retardation effect on the reaction kinetics with an increased FA content has been observed, which not only extended the induction period along with the heat flow evolution but also reduced the cumulative heat release up to 24 h. Spherical FA particles can provide a ball-bearing effect to improve the workability of the hybrid AAM mixtures, while FA also slows down the deterioration of fresh properties since they are less reactive compared to BFS particles. Regarding the strength development, FA results in the reduction at all curing ages in the mixtures with a low silicate modulus (Ms0.25). Similarly, reduction in 1-day compressive strength has been detected in high silicate modulus mixtures (Ms0.5) with FA replacement, while the mixture with 10% FA exhibits the highest compressive strength among Ms0.5 concretes at later curing ages. Bigger capillary pores have been detected in AAM mixtures with an increase in FA content. However, AAM with 10% FA shows the lowest porosity in Ms0.5 mixtures, which is in agreement with the compressive strength results.

This study provides a detailed investigation on the reproducibility of two groups of alkali-activated slag (AAS) mixtures, from both fresh properties and strength development perspectives. Three different commercial sodium silicate solutions and one lab-produced silicate activator (made of silica fume and sodium hydroxide) were used to prepare AAS pastes with the same nominal composition in each group. The reaction process of each AAS mixture was monitored by calorimetry and ultrasonic pulse velocity (UPV) measurements. Meanwhile, mini-slump and flow curve tests measured by rheometer were conducted in the first hour to characterize the evolution of fresh properties. The compressive and flexural strength of hardened AAS mortars were measured at different curing ages. The results revealed that AAS pastes prepared with three different sodium silicate solutions exhibited almost identical reaction kinetics, as well as the evolution of fresh properties and strength development. However, the reaction took place rather fast in AAS pastes made of silica fume. These mixtures showed worse rheology and less strength than the corresponding mixtures prepared with sodium silicate solutions. Furthermore, the present study also showed the feasibility of making the same AAS paste through different class commercial sodium silicate solutions.

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.

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.

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.

The role of capillary pores percolation and gel pores are investigated to explain the underlying differences between relative diffusivity obtained from different experimental techniques using microstructures generated from two different types of hydration model viz., CEMHYD3D (a voxel based approach) and HYMOSTRUC (a vector based approach). These models provide microstructures with different capillary pore connectivity for the same degree of hydration and the same porosity due to the underlying assumptions. In order to account for a C-S-H diffusivity at the micro-scale, a continuum micro-mechanics based model has been proposed. These simulations show that deperolation of capillary pores at around 20% of capillary porosity is essential in order to correctly predict diffusivity of cement paste with water-cement ratio by mass (w/c) in between 0.4 and 0.5. Furthermore from our analysis we present a viable postulate that the higher diffusivity measured by electric resistivity compared to other methods is due to differences in contribution from gel pores. For electrical resistivity measurement it is proposed that all gel pores are diffusive whereas for ion and tracer transport it is proposed that only nitrogen accessible gel pores are diffusive.

This paper provides a comprehensive overview of existing experimental and modelling approaches to determine effective diffusion coefficients of water saturated ordinary Portland cement-based materials. A dataset for diffusivity obtained from different experimental techniques have been presented for cement paste, mortar and concrete. For cement paste at low porosities, diffusivity reported by different authors varies up to a factor of five and electrical resistivity measurements for low capillary porosity are up to one order of magnitude higher compared to other techniques. Experimental data of mortar and concrete reveals predominant influence of increasing tortuosity due to aggregates and limited influence of interface transition zone. Hence, a particular emphasis has been placed on assessing predictability of diffusivity models for cement paste on a larger dataset collected in this paper. It has been observed that all predictive models have similar level of accuracy and fail to predict electrical resistivity data at low capillary porosity as these models are not calibrated using electrical resistivity data.