Generalized structural description of calcium-sodium aluminosilicate hydrate gels: the cross-linked substituted tobermorite model.

Structural models for the primary strength and durability-giving reaction product in modern cements, a calcium (alumino)silicate hydrate gel, have previously been based solely on non-cross-linked tobermorite structures. However, recent experimental studies of laboratory-synthesized and alkali-activated slag (AAS) binders have indicated that the calcium-sodium aluminosilicate hydrate [C-(N)-A-S-H] gel formed in these systems can be significantly cross-linked. Here, we propose a model that describes the C-(N)-A-S-H gel as a mixture of cross-linked and non-cross-linked tobermorite-based structures (the cross-linked substituted tobermorite model, CSTM), which can more appropriately describe the spectroscopic and density information available for this material. Analysis of the phase assemblage and Al coordination environments of AAS binders shows that it is not possible to fully account for the chemistry of AAS by use of the assumption that all of the tetrahedral Al is present in a tobermorite-type C-(N)-A-S-H gel, due to the structural constraints of the gel. Application of the CSTM can for the first time reconcile this information, indicating the presence of an additional activation product that contains highly connected four-coordinated silicate and aluminate species. The CSTM therefore provides a more advanced description of the chemistry and structure of calcium-sodium aluminosilicate gel structures than that previously established in the literature.

Strength Development and Thermogravimetric Investigation of High-Volume Fly Ash Binders.

To address sustainability issues by facilitating the use of high-volume fly ash (HVFA) concrete in industry, this paper investigates the early age hydration properties of HVFA binders in concrete and the correlation between hydration properties and compressive strengths of the cement pastes. A new method of calculating the chemically bound water of HVFA binders was used and validated. Fly ash (FA) types used in this study were sourced from Indonesia and Australia for comparison. The water to binder (w/b) ratio was 0.4 and FA replacement levels were 40%, 50% and 60% by weight. Isothermal calorimetry tests were conducted to study the heat of hydration which was further converted to the adiabatic temperature rise. Thermo-gravimetric analysis (TGA) was employed to explore the chemically bound water (WB) of the binders. The results showed that Australian FA pastes had higher heat of hydration, adiabatic temperature rise, WB and compressive strength compared to Indonesian FA pastes. The new method of calculating chemically bound water can be successfully applied to HVFA binders. Linear correlation could be found between the WB and compressive strength.

Phase evolution of Na2O-Al2O3-SiO2-H2O gels in synthetic aluminosilicate binders.

This study demonstrates the production of stoichiometrically controlled alkali-aluminosilicate gels ('geopolymers') via alkali-activation of high-purity synthetic amorphous aluminosilicate powders. This method provides for the first time a process by which the chemistry of aluminosilicate-based cementitious materials may be accurately simulated by pure synthetic systems, allowing elucidation of physicochemical phenomena controlling alkali-aluminosilicate gel formation which has until now been impeded by the inability to isolate and control key variables. Phase evolution and nanostructural development of these materials are examined using advanced characterisation techniques, including solid state MAS NMR spectroscopy probing (29)Si, (27)Al and (23)Na nuclei. Gel stoichiometry and the reaction kinetics which control phase evolution are shown to be strongly dependent on the chemical composition of the reaction mix, while the main reaction product is a Na2O-Al2O3-SiO2-H2O type gel comprised of aluminium and silicon tetrahedra linked via oxygen bridges, with sodium taking on a charge balancing function. The alkali-aluminosilicate gels produced in this study constitute a chemically simplified model system which provides a novel research tool for the study of phase evolution and microstructural development in these systems. Novel insight of physicochemical phenomena governing geopolymer gel formation suggests that intricate control over time-dependent geopolymer physical properties can be attained through a careful precursor mix design. Chemical composition of the main N-A-S-H type gel reaction product as well as the reaction kinetics governing its formation are closely related to the Si/Al ratio of the precursor, with increased Al content leading to an increased rate of reaction and a decreased Si/Al ratio in the N-A-S-H type gel. This has significant implications for geopolymer mix design for industrial applications.