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Limestone calcined clay cement (LC 3 ) holds promise as a new type of sustainable cement-based material, but the mechanisms underpinning its engineering performance are still poorly understood. Here, a metal intrusion-enhanced imaging approach was employed to quantitatively analyze and link the pore structure development of LC 3  to its hydration process, i.e. solid-phase development, and mechanical performance. We found that the early age microstructural development in LC 3  is inhomogeneous, with the perimeter of limestone particles displaying higher porosity relative to that surrounding calcined clay and clinker. At later ages, the formation of carboaluminates and calcium-aluminate-silicate-hydrates homogenized the overall microstructure of LC 3 , thereby delivering improved mechanical performance. Overall, our analysis suggested a more efficient particle packing in LC 3  mixes, which decreases the volume/connectivity of micro-pores and can account for LC 3 ’s notable flexural strength. These findings can assist the development of improved LC 3  binder formulations alongside other ternary binders with possibly higher limestone additions.

Limestone calcined clay cement: mechanical properties, crystallography, and microstructure development