Basic oxygen furnace slag (SS) is prone to carbonation due to its alkaline properties. The combined use of carbonated basic oxygen furnace slag (CSS) with metakaolin (MK) as a composite supplementary cementitious material (CSS-MK) can improve the reactivity of CSS and significantly lower the overall embodied CO2 emission. However, the impact of CSS-MK on the resistance of external sulfate attack (ESA) of cement remains unclear. This study aims to clarify the influence of CSS-MK on the resistance of cement to ESA. Compressive strength, water absorption, and electrical flux before ESA, and macro-scale expansion, microstructure, and evolution of phase assemblage during ESA were investigated. Results indicate that CSS-MK exhibits higher strength reactivity compared to SS-MK, enabling a 30% cement replacement level without compromising compressive strength after 7 days. CSS-MK reduces water absorption by 37.9% and electrical flux by 67.6%, enhancing transport property and reducing sulfate ion intrusion into the cement paste. The carbonation treatment transforms calcium silicate in SS into CaCO3, decreasing soluble calcium content, and creating a CaCO3-based passivation layer that inhibits sulfate ion corrosion. Meanwhile, the reaction in CSS-MK blends between the CaCO3 in CSS and MK consumes Ca(OH)2, forms ettringite and thermodynamically more stable carboaluminate, and results in the absence of monosulfate prior to ESA and the presence of carboaluminate during ESA, which consequently decreases ettringite content by 40% in paste after 240 days of ESA. Furthermore, at the macroscopic level, the expansion decreased by 85.2% after 360 days of ESA, effectively mitigating specimen cracking and damage.
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