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Precast concrete, cold weather concreting, and the emerging technique of concrete additive manufacturing are applications in which the acceleration of cement hydration plays a critical role. To allow precise control of early cement hydration in these applications, a thorough understanding of the working mechanisms of cement hydration accelerators is required. This study contributes to the understanding of the mechanism by which calcium nitrate (Ca(NO3)2) influences early cement hydration. The influence of Ca(NO3)2 on the hydration of an ordinary Portland cement has been followed by isothermal calorimetry, in situ X‐ray diffraction (XRD), quantitative XRD, compressive strength testing, and the analysis of the pore solution composition. Further, the initial pore solution, the initial phase composition, and the phase composition in the fully hydrated cement have been estimated by thermodynamic calculations to corroborate the experimentally obtained results. The results indicate that Ca(NO3)2, especially at the highest analyzed dosage of 5 wt.%, enhances the formation of ettringite and a nitrate‐containing AFm phase. Furthermore, Ca(NO3)2 accelerates alite hydration. Besides the increased Ca concentration in solution, it has been found that a reduction of the Al concentration in the initial pore solution by Ca(NO3)2 possibly contributes to the accelerating effect of Ca(NO3)2 on alite hydration. [ABSTRACT FROM AUTHOR]

[Display omitted] • Natural and calcined Halloysite clay additives were characterised. • Halloysite clay additives were incorporated to modify AAMs' printing properties. • Enhanced compatibility of calcined Halloysite clay additives in the AAMs was verified. • Buildability and mechanical properties were improved in CH-modified AAMs. This study investigates the effects of natural and calcined halloysite clay minerals ("NH" and "CH", respectively) on the performance of 3D printed alkali-activated materials (AAMs). Halloysite clay minerals are selected as they are low-cost and abundantly available. At first, different characterisation techniques were employed to characterise the NH and CH additives. Mechanical performance, extrusion window, and shape stability of several AAM formulations containing various dosages (0.5 wt% to 5 wt%) of the NH and CH additives were evaluated. The best-performing mixtures in terms of fresh and hardened properties namely, NH-1.5 and CH-1.5 mixtures (containing 1.5 wt% of NH and CH additives, respectively) were then selected for 3D printing. The results showed that the CH-1.5 mixture exhibited enhanced shape stability, buildability, and mechanical properties as compared to the control mixture. The flexural and compressive strengths of 3D printed CH-1.5 samples were 88% and 40%, respectively higher than those of the printed control samples. Using the CH-1.5 mixture, a twisted column with an intricate shape was printed to verify the suitability of the developed CH-modified AAM for the construction of complex structures. This study establishes the use of halloysite clay minerals as low-cost additives for enhancing the mechanical properties and printing performance of AAMs. [ABSTRACT FROM AUTHOR]