Portland cement decalcification and its effects on paste microstructure and mechanical strength have been widely studied. Decalcification in alkali activated slag (AAS) pastes is still not fully understood, however. The present study therefore explored the process in AAS cement pastes, accelerated by submerging specimens in concentrated ammonium nitrate solutions (NH4NO3) for 3–21 days to induce leaching. Two AAS pastes were prepared with slag of different origins (Spanish and Colombian) and chemical compositions. OPC pastes were used as a reference. The findings showed that decalcification has a more adverse impact on OPC than AAS pastes strength. BSEM/EDX and 29Si MAS NMR data nonetheless confirmed that Ca leaches out of C–A–S–H gels (formed in AAS pastes) to an extent that depends on the nature of the prime material. OPC pastes were shown to generate more silica gel with a very low Ca content (Q3 and Q4 units). Moreover, the higher the percentage of such units, the lower was mechanical strength. Decalcification in slag with lower MgO and higher Al2O3 contents leads to the formation of smaller amounts of silica gel. The resulting gel was more compact and stable due to more intense chain cross-linking a possible tri-dimensional structure.
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