Autogenous and Chemical Shrinkage of Limestone Calcined Clay Cement (LC3) Pastes

This study investigated the chemical and autogenous shrinkage behaviour of limestone calcined clay cement (LC3) pastes incorporating calcined clays sourced from Australia, France, and India. Hydration development and microstructural evolution were examined using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and pore-size distribution analysis. Results showed that LC3 mixes hydration accelerates during early phases, with the main silicate hydration peak appearing more prominently than that in the GP and FA reference pastes, indicating increased nucleation and growth of hydration products due to the limestone filler effect. LC3 pastes exhibited higher autogenous shrinkage overtime, strongly influenced by calcined clay reactivity and particle fineness. A clear correlation was observed between pore refinement and autogenous deformation during the early phases (7 days): pastes with a greater volume of fine pores showed higher early-age autogenous shrinkage during the first 7 days of hydration. In contrast, the chemical shrinkage of LC3 mixes was comparable to that of the GP and FA systems at early ages (≤7 days) but became lower after 28 days, attributed to both the matrix densification and additional nucleation sites provided by the limestone. Overall, LC3 reduces long-term chemical shrinkage and densifies the microstructure; however, the refined pore structure and increased internal water demand lead to higher autogenous shrinkage. These findings demonstrate a direct link between hydration-driven microstructural evolution (phase formation and pore refinement) and the resulting shrinkage behaviour.