ii The nature of the calcium-silicate-hydrate phase in hydrated Portland cement has been the subject of considerable debate for decades. Various nanostructural models have been proposed including those constructed from colloidal-based particulate systems and those formulated on the basis of layered calcium-silicate-hydrates. These are examined in detail in the literature review section of the thesis. Relatively recent composition-based models have been proposed by Taylor and Richardson-Groves. These models contain structural elements comprised of 1.4 nm tobermorite and jennite. Details are also provided in the literature review. There is however a paucity of data on the engineering properties of pure calcium-silicate-hydrate phases and virtually none on the mechanical performance of 1.4 nm tobermorite and jennite. The global objective of this thesis was to examine the compatibility of the composition-based models with the engineering behaviour of the pure tobermorite and jennite phases. Pure phases of a variety of layered calcium-silicate-hydrates were synthesized and novel techniques developed to determine their engineering characteristics in a variety o
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