Time-dependent phase quantification and local structure analysis of hydroxide-activated slag via X-ray total scattering and molecular modeling

TL;DR

This paper presents a combined atomistic modeling and X-ray scattering approach to quantify phase transformations in hydroxide-activated slag over time, providing detailed insights into its structural evolution.

Contribution

It introduces a novel method integrating molecular dynamics and PDF analysis to quantify phases and reaction degree in GGBS during activation.

Findings

DOR follows a logarithmic trend up to 5 months.

Early age DOR fits a modified pseudo-single step reaction model.

Results agree with calorimetry, FTIR, and neutron scattering data.

Abstract

Here, an approach to quantify the amorphous-to-disordered/crystalline transformation occurring in NaOH-activated ground granulated blast-furnace slag (GGBS) is outlined that combines atomistic modeling with in situ pair distribution function (PDF) analysis. Firstly, by using force-field molecular dynamics (MD) simulations, a detailed structural representation is generated for the amorphous GGBS that is in agreement with experimental X-ray scattering data. Use of this structural representation along with literature-derived structures for the reaction products allows for real space X-ray PDF refinement of the alkaline activation of GGBS, resulting in the quantification of all phases and the degree of reaction (DOR) as a function of reaction time. All phases and the DOR are seen to approximately follow a logarithmic-type time-dependent behavior up to 5 months, while at early age (up to 11 hours) the DOR is accurately captured by a modified pseudo-single step first-order reaction model. Lastly, the evolution of DOR is found to agree with several other complementary in situ data containing quantitative reaction information, including isothermal conduction calorimetry, Fourier transform infrared spectroscopy, and quasi-elastic neutron scattering.