Factors Affecting Synthesized C-S-H CO2 Uptake: Initial Alkalinity and Ca/Si

The dynamic evolution of alkalinity during hydration/carbonation of CO2-conditioned cements results in the formation of polymorphic hydrated calcium silicates (C-S-H), whose differences in carbon sequestration capacity have not been systematically investigated. However, the micro-nano structures and carbon sequestration capacities of C-S-H are controlled by the dynamic effects of pore solution alkalinity and Ca/Si. Accordingly, different alkalinity and Ca/Si were set to simulate the cement hydration environment for the synthesis of C-S-H, and tests such as thermogravimetric and 29Si nuclear magnetic resonance (NMR) were used to investigate the effects and mechanisms of initial alkalinity and Ca/Si on the morphology of the synthesized C-S-H, the CO2 uptake. The results showed that the C-S-H synthesized at pH 7.2–12.0 and Ca/Si ratio of 1.0–2.3 was in flocculated and acicular forms, which were well crystallized and dominated by Q2, while its CO2 uptake was positively correlated with Ca/Si. On the contrary, the synthesized C-S-H was poorly crystallized under the conditions of pH increasing to 13.5 and Ca/Si ratios of 1.0–2.3. With the increase in Ca/Si, the synthesized C-S-H evolved from Q2-dominated foil to Q1-dominated porous structure, and its CO2 uptake was non-positively correlated with Ca/Si. This was mainly related to the average pore diameter of C-S-H and its silica-oxygen tetrahedral structure. This was mainly related to the average pore diameter of C-S-H and its silica-oxygen tetrahedral structure.