Systematic manipulation of the reactivity
of silicate materials
in aqueous environment remains a challenging topic. Herein, by combining
first-principles and reactive molecular dynamics simulations, we present
a complete picture of the influence of impurity species on hydration
reactivity, using the reactive triclinic tricalcium silicate phase
as an example. We show that although initial hydration is influenced
by the surface’s chemistry and structure, longer-term hydration
is primarily controlled by proton transport through the bulk solid.
Both shorter- and longer-term hydration processes are noted as being
intrinsically correlated with electronic features. These outcomes
provide the first direct evidence of the linkages between electronic
structure and the longer-term (i.e., on the order of several nanoseconds)
hydration behavior and sensitivity of hydrophilic crystalline materials
and also offer a pathway to efficient compositional design for similar
materials