Tuning the Carbonation Resistance of Metakaolin–Fly Ash-Based Geopolymers: The Dual Role of Reactive MgO in Microstructure and Degradation Mechanisms

Geopolymers, as a novel class of low-carbon and eco-friendly cementitious material, exhibit outstanding durability and promote the resource utilization of industrial solid wastes. However, as a promising alternative to ordinary Portland cement, its susceptibility to carbonation-induced degradation may limit its widespread application. To address this challenge, this study systematically examined the effects of magnesium oxide (MgO) content and the metakaolin-to-fly ash ratio on the carbonation performance, mechanical properties, pH value, and microstructures of metakaolin–fly ash-based (MF-based) geopolymer pastes. The findings revealed that an increase in the fly ash ratio correlated with a decline in the compressive strength of MF-based geopolymer pastes. Conversely, the incorporation of MgO significantly enhanced the compressive strength, with higher fly ash ratios leading to more substantial improvements in strength. Furthermore, the addition of MgO and fly ash effectively mitigated the penetration of carbonation and the associated decrease in the pH value of the MF-based geopolymer pastes. Specifically, compared to the control group without MgO (M8F2-0%), MF-based geopolymer pastes with 4% and 8% MgO additions exhibited reductions in carbonation depth of 69.4% and 80.4%, respectively, after 28 days of carbonation, while pH values were observed to be 1.22 and 1.15 units higher, respectively. Additionally, microscopic structural analysis revealed that the inclusion of MgO resulted in a reduction in pore size, porosity, and mean pore diameter within the geopolymer pastes. This improvement was mainly attributed to the promotion of hydration processes by MgO, leading to the formation of fine Mg(OH)2 crystals within the high-alkalinity pore solution, which enhances microstructural densification. In conclusion, the incorporation of MgO significantly improves the carbonation resistance and mechanical performance of MF-based geopolymers. It is recommended that future studies explore the long-term performance under combined environmental actions and evaluate the economic and environmental benefits of MgO-modified geopolymers for large-scale applications.