Compressive reactive molecular dynamics on mechanical and structural behaviors of geopolymers: Imposing lateral constraints and varied temperatures

Geopolymer concrete offers superior mechanical properties and microstructure, yet micro-level compressive properties and structural evolutions remain insufficiently understood. This study employed molecular dynamics to simulate the uniaxial compressions of the sodium aluminosilicate hydrate (N-A-S-H) under UCZ, BCZ, and TCZ (z-axial compressions with zero, one, and two dimensions restrictions, respectively) conditions at 263 K, 300 K, and 800 K. The results provided valuable insights linking mechanical behavior with structural properties. Stress fluctuations in the yield stage were attributed to the continuous formation and fracture of Al-O-H bonds during micro-molecule processes. In the later compression stages, the rapid increase in Si-O-H groups suggested that water molecules equally attacked Al and Si tetrahedra due to limited voids. Under UCZ and BCZ conditions, slight bond contraction occurred, with the main structural resistance arising from bond angle bending within the skeleton. In contrast, TCZ experienced notable changes in both bond lengths and bond angles due to bilateral displacement constraints. The evolutionary molecular processes exhibited insensitive response to the temperature, especially under TCZ conditions. Additionally, varying trends were observed in different bond-angle styles (e.g., within or inside tetrahedra), providing a crucial insight for the design of N-A-S-H to determine optimal components.