The synthesis of N-A-S-H gel with high Si/Al ratios (>2) has been rarely reported in the literature, leaving the establishment of a reliable synthesis route as an open challenge. This paper aims to synthesize N-A-S-H gels with Si/Al ratios ranging from 1 to 3 and establish their thermodynamic database. The effects of reaction temperature, reaction time, initial Si/Al, concentration of reactants and pH of the matrix on the Si/Al ratios of the synthesized N-A-S-H gel were investigated. Results showed that N-A-S-H gels with target Si/Al ratios can be synthesized by controlling the concentration of reactants, pH and initial Si/Al ratios. The solubility products of the obtained N-A-S-H gels were determined via dissolution tests at different temperatures, to determine thermodynamic data. The development of this experimentally derived thermodynamic database of N-A-S-H gels constitutes a crucial step in the advancement of thermodynamic modeling of geopolymer, providing valuable insight into geopolymer reactions and phase assemblages.

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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.

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Many (inter)national standards exist to evaluate the resistance of mortar and concrete to carbonation. When a carbonation coefficient is used for performance comparison of mixtures or service life prediction, the applied boundary conditions during curing, preconditioning and carbonation play a crucial role, specifically when using latent hydraulic or pozzolanic supplementary cementitious materials (SCMs). An extensive interlaboratory test (ILT) with twenty two participating laboratories was set up in the framework of RILEM TC 281-CCC ‘Carbonation of Concrete with SCMs’. The carbonation depths and coefficients determined by following several (inter)national standards for three cement types (CEM I, CEM II/B-V, CEM III/B) both on mortar and concrete scale were statistically compared. The outcomes of this study showed that the carbonation rate based on the carbonation depths after 91 days exposure, compared to 56 days or less exposure duration, best approximates the slope of the linear regression and those 91 days carbonation depths can therefore be considered as a good estimate of the potential resistance to carbonation. All standards evaluated in this study ranked the three cement types in the same order of carbonation resistance. Unfortunately, large variations within and between laboratories complicate to draw clear conclusions regarding the effect of sample pre-conditioning and carbonation exposure conditions on the carbonation performance of the specimens tested. Nevertheless, it was identified that fresh and hardened state properties alone cannot be used to infer carbonation resistance of the mortars or concretes tested. It was also found that sealed curing results in larger carbonation depths compared to water curing. However, when water curing was reduced from 28 to 3 or 7 days, higher carbonation depths compared to sealed curing were observed. This increase is more pronounced for CEM I compared to CEM III mixes. The variation between laboratories is larger than the potential effect of raising the CO₂ concentration from 1 to 4%. Finally, concrete, for which the aggregate-to-cement factor was increased by 1.79 in comparison with mortar, had a carbonation coefficient 1.18 times the one of mortar.

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New self-healing agents that can chemically bind seawater ions invading cracked cementitious materials were proposed. The potential of self-healing and binding of seawater ions were investigated by thermodynamic modeling. It was found that CaO-NaAlO₂ and CaO-metakaolin agents can have Cl⁻, SO₄²⁻ and Mg²⁺ chemically bound by reacting with sea water to form Friedel's salt, Kuzel's salt, ettringite and hydrotalcite. The removal of Cl⁻ from seawater firstly increased and then decreased with the increase of Ca/Al molar ratio in both agents, while the removal of Mg²⁺ and SO₄²⁻ were hardly influenced and approximated 100%. Because NaAlO₂ dissolves and releases Al(OH)₄⁻ rapidly, precipitates binding Cl⁻, SO₄²⁻ and Mg²⁺ were formed fast. In comparison, the reaction of metakaolin binding aggressive ions occurred after 3 days. Because of the faster reaction and the capacity to make [Cl⁻]/[OH⁻] lower in the solution, CaO-NaAlO₂ would be more efficient for self-healing and mitigating reinforcement corrossion than CaO-metakaolin.

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The article “Understanding the carbonation of concrete with supplementary cementitious materials: a critical review by RILEM TC 281-CC”, written by Stefanie von Greve-Dierfeld, Barbara Lothenbach, Anya Vollpracht, Bei Wu, Bruno Huet, Carmen Andrade, César Medina, Charlotte Thiel, Elke Gruyaert, Hanne Vanoutrive, Isabel F. Saéz del Bosque, Ivan Ignjatovic, Jan Elsen, John L. Provis, Karen Scrivener, Karl-Christian Thienel, Kosmas Sideris, Maciej Zajac, Natalia Alderete, Özlem Cizer, Philip Van den Heede, Robert Douglas Hooton, Siham Kamali-Bernard, Susan A. Bernal, Zengfeng Zhao, Zhenguo Shi and Nele De Belie was originally published electronically on the publisher’s internet portal on 22 October 2020 without open access. The copyright of the article changed in February 2021 to © The Author(s) 2021 and the article is forthwith distributed under the terms of the Creative Commons Attribution 4.0 International License, which permits use, duplication, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license and indicate if changes were made.@en

Blended cements, where Portland cement clinker is partially replaced by supplementary cementitious materials (SCMs), provide the most feasible route for reducing carbon dioxide emissions associated with concrete production. However, lowering the clinker content can lead to an increasing risk of neutralisation of the concrete pore solution and potential reinforcement corrosion due to carbonation. carbonation of concrete with SCMs differs from carbonation of concrete solely based on Portland cement (PC). This is a consequence of the differences in the hydrate phase assemblage and pore solution chemistry, as well as the pore structure and transport properties, when varying the binder composition, age and curing conditions of the concretes. The carbonation mechanism and kinetics also depend on the saturation degree of the concrete and CO₂ partial pressure which in turn depends on exposure conditions (e.g. relative humidity, volume, and duration of water in contact with the concrete surface and temperature conditions). This in turn influence the microstructural changes identified upon carbonation. This literature review, prepared by members of RILEM technical committee 281-CCC carbonation of concrete with supplementary cementitious materials, working groups 1 and 2, elucidates the effect of numerous SCM characteristics, exposure environments and curing conditions on the carbonation mechanism, kinetics and structural alterations in cementitious systems containing SCMs.

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