Molecular Insight into the Structural and Mechanical Properties of Ca-Based Geopolymers

Ca-based geopolymers are a principal product of introducing calcium into geopolymers. Analyzing Ca-based geopolymers structural and mechanical properties aids in optimizing mix design of geopolymers. In this paper, partially reacted low-polymerization and fully reacted high-polymerization models were constructed to examine the structural and mechanical properties of Ca-based geopolymers with varying calcium contents via molecular dynamics simulations. Results show that Ca-based geopolymers contain pentacoordinate aluminum and tricluster oxygen which is more brittle and makes the structure loose. In low-polymerization models, an increase in calcium content accelerates the polymerization rate by overcoming the low-temperature reaction barrier. However, calcium content hinders the formation of pentacoordinate aluminum, decreasing the final degree of polymerization, resulting in weakened mechanical properties. In high-polymerization models, increased calcium decreases tricluster oxygen content, resulting in improved mechanical properties. While the hydrolysis reaction reduces mechanical properties, the weakening effect of water is greater than the enhancing effect of calcium.