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M-S-H gels were synthesised via reaction of Mg(OH)2 with silica fume, cured at 35 °C for up to 112 days, and their chemical and nanostructural evolution was examined. M-S-H gels with structural similarity to the thermodynamically stable serpentine-group mineral lizardite were formed. Quantification of 25Mg and 29Si MAS and 1H 29Si CPMAS NMR, electron microscopy, and thermogravimetric data showed dissolution of brucite and silica fume, and M-S-H formation, all occurred linearly with time up to 56 days. Data showed strong correlation with the Avrami-Erofeyey nucleation kinetic model, indicating M-S-H formation was governed by nucleation reactions. After 112 days, two distinct M-S-H gels were formed: a Si-rich M-S-H gel with molar Mg/Si = 0.55(±0.2), and a Mg-rich M-S-H gel with molar Mg/Si = 0.80(±0.5). Nanostructural rearrangement of M-S-H continues up to 112 days, with increased crosslinking and polymerisation. This new insight is important for application of M-S-H binders in both construction and radioactive/toxic waste immobilisation.
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