Insights into the impact of small anionic additives on Mg-silicate hydrate nucleation

Abstract

Magnesium silicate (MS) cement, which uses magnesium silicate hydrate (M-S-H) as its primary binding phase, is a promising low-carbon alternative to Portland cement. However, the slow dissolution of MgO limits the release of Mg ions, which is critical for the formation of M-S-H. To address this issue, solubilizers that complex Mg²⁺ and promote MgO dissolution have been proposed, provided that they do not significantly hinder M-S-H formation. This study systematically examined the effects of four anionic additives-acetate, citrate, orthophosphate, and carbonate-on M-S-H nucleation and early growth, developing a highly reproducible crystallization scenario. The observed reduction in supersaturation at the nucleation point for specific additive concentrations suggests that Mg-anion complexes may play an active role in M-S-H nucleation, potentially allowing M-S-H to form at lower supersaturation levels, which could be beneficial for MS cement applications. However, as shown here, additives such as citrate, while not inhibiting nucleation, can significantly slow the growth of M-S-H, potentially compromising the strength development of MS cement. Among the additives studied, moderate concentrations of phosphate and carbonate show the most promise, as they have minimal effects on the formation process while potentially reducing the supersaturation for M-S-H nucleation. Although further research is necessary to fully understand the effects of these anions, this study provides valuable insights into their impact on M-S-H nucleation and early growth.