Influence of Alkalis on Natural Carbonation of Limestone Calcined Clay Cement Pastes

Abstract

Vulnerability to atmospheric carbonation is one of the major durability concerns for limestone calcined clay cement (LC3) concrete due to its relatively low overall alkalinity. In this study, the natural carbonation behaviors of ternary ordinary Portland cement-metakaolin-limestone (OPC-MK-LS) blends containing various sulfate salts (i.e., anhydrous CaSO4, Na2SO4, and K2SO4) are studied, with the aim of revealing the influence of alkali cations (Na+, K+). Detailed analyses on the hydrated phase assemblage, composition, microstructure, and pore structure of LC3 pastes prior to and post indoor carbonation are conducted. The results show that the incorporation of sulfate salts accelerates the setting and strength gain of LC3 pastes, likely through enhancement of ettringite formation, but undermines its later age strength achievement due to the deleterious effect of alkali cations (Na+, K+) on late age OPC hydration. The carbonation resistance of LC3 systems is considerably undermined, particularly with the incorporation of Na2SO4 or K2SO4 salts, due to the simultaneous pore coarsening effect and reduced CO2-binding capacity. The carbonation-induced phase and microstructural alterations of LC3 pastes are discussed and compared with those of reference OPC pastes.