Development of physics-based compositional parameters for predicting the reactivity of amorphous aluminosilicates in alkaline environments

TL;DR

This study introduces two physics-based compositional parameters, derived from molecular dynamics and topological theory, to predict the reactivity of amorphous aluminosilicates in alkaline environments, outperforming existing methods.

Contribution

It presents novel, directly calculable parameters linking aluminosilicate composition to reactivity, advancing predictive capabilities in materials science.

Findings

Modified AMODE parameter outperforms existing predictors.

Topology constraint parameter effectively describes glass reactivity.

Parameters are derived directly from chemical composition.

Abstract

The reactivity of amorphous aluminosilicates in alkaline environments is important to many applications, including blended Portland cements and alkali-activated materials (AAMs). Here, two physics-based compositional parameters are derived to describe the relative reactivity of CaO-Al2O3-SiO2 and CaO-MgO-Al2O3-SiO2 glasses in alkaline environments: (i) a modified average metal oxide dissociation energy (AMODE) parameter developed from molecular dynamics simulations; and (ii) a topology constraint parameter derived from topological constraint theory. Both parameters are seen to generally outperform existing compositional parameters from the literature for a wide range of aluminosilicate glasses. Given that both the modified AMODE and topology constraint parameters can be calculated directly from chemical compositions, this study represents a major step forward in connecting aluminosilicate glass compositions with their reactivity in alkaline environments. The limitations of these compositional parameters, including their inability to capture the impact of Ca versus Mg on glass reactivity, have also been discussed.