Loess, a terrestrial clastic sediment, is formed essentially by the accumulation of wind-blown dust, while stone waste (SW) is an industrial waste produced during stone machining. Utilising loess and SW to prepare environmentally-friendly supplementary cementitious materials can not only address environmental issues caused by solid waste landfills but also meet the demand of reinforcement of coal-seam floor aquifer for grouting materials. In this paper, the effects of the loess/SW mass ratio and calcination temperature on the transformation of calcined products are investigated and their pozzolanic activities are evaluated. The workability, environmental impact and cost of grouting materials based on cement and calcined products are also assessed. Experimental results reveal that higher temperatures favour the formation of free lime and periclase, which tend to be involved in solid-state reactions. Higher temperature and loess/SW mass ratio strengthens the diffraction peaks of dodecalcium hepta-aluminate (C12A7), dicalcium ferrite (C2F) and dicalcium silicate (C2S). The clay minerals in loess become completely dehydroxylated before 825 °C, generating amorphous SiO2 and Al2O3. Covalent Si–O bonds are interrupted and that disordered silicate networks are generated in the calcined products, which is confirmed by the increased strength of the Si29 resonance region at −60 ppm to −80 ppm. Although co-calcined loess and SW contain the most four-fold aluminium at 950 °C, recrystallisation depresses the pozzolanic activity. Hence, the loess/SW sample designated LS2-825 exhibits the better hydration activity. Additionally, grouting materials composed of cement and LS2-825 exhibit good setting times, fluidity, strength and a low carbon footprint in practical engineering applications, and they also provide the additional benefit of being cost effective.
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