Effect of calcite filler on carbonation behavior in a synthesized C‐S‐H binder

Abstract Widespread implementation of portland limestone cements (PLC) in industry has raised new questions about their carbonation resistance due to higher initial limestone content than ordinary portland cement. While carbonation of portland cement and each of its hydrate phases has been studied at a fundamental level, the integral role of how limestone fillers interact chemically or physically during carbonation necessitates further study. In this study, a C‐S‐H binder comprised of a highly reactive zeolite pozzolan and lime was used to evaluate the effect of varying calcite additions on carbonation behavior at a microstructural level. Fundamental insight into hydration kinetics and carbonation mechanisms of hydraulic binders was obtained via analysis of the C‐S‐H and calcite microstructure. X‐ray microcomputed tomography (X‐ray CT) was used to quantify microstructural changes, and the results showed a decrease in shrinkage for increased calcite dosages, with a ∼50% reduction observed for a 45% wt. calcite replacement level. Crystallographic and thermal analyses measured compositional changes in the binder and confirmed that shrinkage was related to the decalcification of C‐S‐H. The addition of calcite to the C‐S‐H binder effectively reduced the liquid‐to‐solid ratio, porosity, and amount of C‐S‐H present in these binders. Ultimately, these results help elucidate how the carbonation risks of PLC can be mitigated by proportioning the mixture water only to the reactive component of the binder.