Coal-fired slag (CFS) is one of the significant solid wastes generated in the process of coal development and utilization. There are obvious differences in the properties of CFS with different particle sizes after high-temperature melting, which affects its quality and limits its high-value application, exacerbating the contradiction between development and the environment. This study investigates the activity differences among various graded CFS and establishes a relationship between CFS particle size and its performance. Utilizing CFS as precursor, we explored the relationship between the macroscopic properties of modified magnesium slag-activated CFS cementitious material (CFS·C) and CFS activity. Physicochemical and activity assessments reveal that the pozzolanic activity (K and API values) of CFS across different particle sizes initially increases before decreasing with size increment, correlating positively and negatively with the contents of Si, Al, and Fe oxides and loss on ignition (LOI), respectively. Specifically, CFS with particle sizes <0.15 mm (S1) exhibited the lowest activity, impacting the overall activity of CFS, whereas sizes between 0.3 ∼ 1.18 mm (S3) demonstrated the highest activity. The hydration heat, mechanical properties and microstructural analyses of CFS·C correspond with these activity trends. CFS·C of S1 displayed the worst mechanical properties (3.61 MPa), minimal cumulative exothermic and thermogravimetric total mass loss (13.42 J/g and 2.81%), and a loose and porous structure. Conversely, CFS·C of S3 presented the highest 28 d strength (7.21 MPa), maximal cumulative exothermic and thermogravimetric total mass loss (17.2 J/g and 6.45%), and a dense microstructure. Correlation analyses confirm that Si, Al, and Fe oxides content, LOI, pozzolanic activity, cumulative heat release and thermogravimetric total mass loss effectively predict 28 d strength trends. In conclusion, enhancing the proportion of CFS particles above 0.15 mm in the discharge process could significantly improve the overall cementitious performance of CFS and promote its high-value utilization, thereby mitigating associated emission pollution issues.
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