Fly ash which encompasses a mixture of glassy and crystalline aluminosilicates is an abundant supplementary cementitious material (SCM), valuable for replacing ordinary portland cement (OPC) in the binder fraction in concrete. Because higher OPC replacement levels are desired, it is critically important to better understand and quantify fly ash reactivity. By combining molecular dynamics (MD) simulations and vertical scanning interferometry (VSI), this study establishes that the reactivity of the glassy fractions in a fly ash with water (i.e., their aqueous dissolution rate) is controlled by the number of constraints placed on atoms within the disordered aluminosilicate network. More precisely, an Arrhenius-like dependence of dissolution rates on the atomic network topology is observed. Such topological controls on fly ash reactivity are highlighted for a range of U.S. commercial fly ashes spanning CaO-enriched and SiO2-enriched compositions. The structure-property relationships reported herein establish an improved framework to control and estimate fly ash-cement interactions in concrete.

Calcium hydroxide (Ca(OH)₂), a commodity chemical, finds use in diverse industries ranging from food, to environmental remediation and construction. However, the current thermal process of Ca(OH)₂ production via limestone calcination is energy- and CO₂-intensive. Herein, we demonstrate a novel aqueous-phase calcination-free process to precipitate Ca(OH)₂ from saturated solutions at sub-boiling temperatures in three steps. First, calcium was extracted from an archetypal alkaline industrial waste, a steel slag, to produce an alkaline leachate. Second, the leachate was concentrated using reverse osmosis (RO) processing. This elevated the Ca-abundance in the leachate to a level approaching Ca(OH)₂ saturation at ambient temperature. Thereafter, Ca(OH)₂ was precipitated from the concentrated leachate by forcing a temperature excursion in excess of 65 °C while exploiting the retrograde solubility of Ca(OH)₂. This nature of temperature swing can be forced using low-grade waste heat (≤100 °C) as is often available at power generation, and industrial facilities, or using solar thermal heat. Based on a detailed accounting of the mass and energy balances, this new process offers at least ≈65% lower CO₂ emissions than incumbent methods of Ca(OH)₂, and potentially, cement production.