The high alkalinity and low hydraulic reactivity of red mud (RM) severely restrict its application in cement or concrete industry. In this study, an innovative CO2 mineralization approach for simultaneous alkalinity neutralization and reactivity enhancement of RM was developed, aiming to promote its use as a supplementary cementitious material (SCM). The results demonstrate that CO2 mineralization significantly mitigates the alkalinity of RM, reducing the pH from 12.65 to 7.59. The carbonated RM exhibited remarkable pozzolanic activity, with a strength activity index of 113 % (7-day) and 109.8 % (28-day), confirming its potential as a highly active SCM. The carbonation of RM demonstrated exceptional CO2 sequestration capacity, capturing 24.34 g of CO2 per 100 g of RM, achieving a carbonation degree of 62.89 %. Alkalinity neutralization primarily occurs through carbonation reactions between CO2 and alkaline components, generating stable carbonate precipitates. Furthermore, carbonation kinetics analysis revealed a 60.5 % reduction in average particle size and a 235.1 % increase in specific surface area of RM, indicating significant microstructural refinement. Rapid carbonation of C3S, C2S, sodalite, perovskite and jennite to the formation of calcite, metastable CaCO3 and silica-alumina gel, indicating mineral reconfiguration of RM. The combined effects of microstructure refinement and mineral reconfiguration jointly enhanced the pozzolanic activity of RM. Overall, these findings establish RM carbonation as a dual-purpose solution for sustainable waste valorization and carbon capture, offering both technical and environmental advantages for industrial implementation.
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