Modeling the Early Stage Formation Mechanisms of Calcium Silicate Hydrates and Related Gels

TL;DR

This study uses computational modeling to uncover the fundamental early-stage mechanisms of calcium silicate hydrate gel formation in cement, aiming to enable innovations that could reduce CO2 emissions and improve concrete durability.

Contribution

It introduces a computational approach to simulate and analyze the formation mechanisms of cement hydrates at the molecular level, providing new insights into early-stage gel formation processes.

Findings

Identified dominant mechanisms controlling gel formation.

Simulated high pH pore solution chemistry accurately.

Provided insights for materials engineering improvements.

Abstract

Arguably the most ubiquitous construction material in modern civilization, concrete is enabling the development of megacities around the globe together with increasing living standards in developing nations. However, it can be argued that the concrete industry's somewhat empirical and conservative approach to change is hampering innovation and associated CO2 reductions, yet materials engineering of the essential phase(s) responsible for strength and durability would enable for revolutionary advancements to be achieved. Using a computational materials engineering approach, we simulate the fundamental solution-based building blocks of cement hydrates and their propensity to form larger complexes as assessed from Gibbs free energies of chemical reactions characteristic of the formation of calcium-silicate-hydrate, calcium-alumino-silicate-hydrate and sodium-containing calcium-alumino-silicate-hydrate gels. By accurately simulating the high pH pore solution chemistry in Portland cements and related systems, along with discrete solvation of the species, we discover and discuss the dominant early stage mechanisms controlling gel formation in these systems.