In this study, we investigated the impact of aluminium ion (Al3+) incorporation on the microstructure and the phase transformation of the magnesium silicate hydrate system. The magnesium silicate hydrate system with aluminium was prepared by mixing magnesium oxide and silica fume with different aluminium ion contents (the Al/Si molar ratios of 0.01, 0.02, 0.05, 0.1, 0.2) at room temperature. The high degree of polymerization of the magnesium silicate hydrate phases resulted in the limited incorporation of aluminium in the structure of magnesium silicate hydrate. The silicon-oxygen tetrahedra sites of magnesium silicate hydrate layers, however, were unable to substitute for silicon sites through inverted silicon-oxygen linkages. The increase in aluminium ion content raised the degree of polymerization of the magnesium silicate hydrate phases from 0.84 to 0.92. A solid solution was formed from residual aluminum-amorphous phases such as hydroxyl-aluminum and magnesium silicate hydrate phases. X-ray diffraction (XRD), field emission scanning electron microscope (F-SEM), and 29Si and 27Al MAS NMR data showed that the addition of Al3+ promotes the hydration process of MgO and has an obvious effect on the appearance of M-S-H gel. The gel with low aluminum content is fluffy, while the gel with high aluminum content has irregular flakes. The amount of Al3+ that enters the M-S-H gel increased with the increase of Al3+ content, but there was a threshold: the highest Al/Si molar ratio of M-S-H gel can be maintained at about 0.006.

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The current investigation focuses on the stability of the magnesium oxide-based cementitious system under the action of sulfate attack and the dry-wet cycle. The phase change in the magnesium oxide-based cementitious system was quantitatively analyzed by X-ray diffraction, combined with thermogravimetry/derivative thermogravimetry and scanning electron microscope, to explore its erosion behavior under an erosion environment. The results revealed that, in the fully reactive magnesium oxide-based cementitious system under the environment of high concentration sulfate erosion, there was only magnesium silicate hydrate gel formation and no other phase; however, the reaction process of the incomplete magnesium oxide-based cementitious system was delayed, but not inhibited, by the environment of high-concentration sulfate, and it tended to turn completely into a magnesium silicate hydrate gel. The magnesium silicate hydrate sample outperformed the cement sample, in terms of stability in a high-concentration sulfate erosion environment, but it tended to degrade considerably more rapidly, and to a greater extent, than Portland cement, in both dry and wet sulfate cycle environments.