The accumulation of coal gangue poses significant environmental challenges due to its massive volume and low reactivity. This study investigates the influence of calcium hydroxide (Ca(OH)₂) and gypsum on the mechanical properties, hydration, and pore structure of low-carbon cementitious materials incorporating high volumes of calcined coal gangue (CCG) and limestone. The results showed that the addition of Ca(OH)₂ significantly increased compressive strength, with a 19 % improvement at 28 days in LCC-40-P mix, which contained 40 % cement and 2.73 % Ca(OH)₂ by weight. The incorporation of 10 % gypsum in the LCC-40-P mix and 20 % gypsum in the LCC-70 mix (containing 70 % cement without Ca(OH)₂) effectively refined the pore structure, reduced overall porosity, and enhanced the material's density and mechanical properties, resulting in compressive strengths of 38.4 MPa (72 % of the strength of Portland cement) and 50.2 MPa (94 % of the strength of Portland cement) at 28 days, respectively. Microstructure and hydration heat tests showed that the addition of Ca(OH)₂ accelerates the hydration reaction and significantly enhanced compressive strength by ensuring sufficient Ca(OH)₂ for pozzolanic reactions, leading to the formation of additional calcium silicate hydrate, calcium aluminate silicate hydrate and carboaluminate phases. Gypsum refined the pore structure by shifting the pore size distribution towards smaller sizes, reducing overall porosity, and increasing the proportion of gel and small capillary pores. These findings highlight the potential of using CCG with optimized additives to develop sustainable, low-carbon construction materials with enhanced performance characteristics.
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