Key Takeaways & Executive Findings
- •• First-principles DFT study reveals that multiple water molecule adsorption on M3-C3S(001) exhibits anticooperative behavior, with total adsorption energy becoming more negative but average adsorption energy per molecule becoming more positive as coverage increases. • Water–water interactions weaken water–surface interactions, highlighting the need to consider coverage effects in modeling cement hydration. • Dissociative adsorption, forming Ca–OH bonds, facilitates calcium detachment from covalent oxygen, providing atomic-level insights into the initial hydration mechanism. • The findings extend understanding from single to multiple water molecule adsorption, crucial for optimizing cement strength development and sustainable construction materials.
Abstract
An in-depth understanding of the hydration mechanism of tricalcium silicate is an important basis for optimizing cement strength development. In this study, the adsorption of water molecules onto the M3-C3S(001) surface at different water coverage levels (θ = 1/5, 2/5, 3/5, 4/5, and 1) was investigated using first-principles calculations. The results demonstrate that the conclusions obtained for single water molecule adsorption cannot be fully applied to multiple water molecule adsorption. The total adsorption energies become more negative with increasing water coverage, while the average adsorption energy of each water molecule becomes more positive with increasing water coverage. The water–water interactions reduce the water–surface interactions and are responsible for the anticooperative adsorption of multiple water molecules onto M3-C3S(001). The formation of Ca–OH (–Ca) bonds favors the detachment of Ca from covalent oxygen, which reveals the significant role of dissociative adsorption. This work aims to extend the water adsorption study on M3-C3S(001) from single water molecule adsorption to multiple water molecule adsorption, providing more detailed insights into the initial water reaction on the C3S surface.
1. Introduction
Cement, the most important material in the world [1–4], is widely used in civil engineering projects, such as roads, houses, and bridges, in the form of concrete formed by its mixing with water and aggregates [5]. It is considered the second most consumed substance in the world after water [6]. In 2021, global cement production has reached 4.4 billion tonnes [7]. Driven by population growth, urbanization, and accelerated public infrastructure development, the demand for cement will continue to increase [5]. It is expected that global cement production will grow to 4 billion tonnes–8 billion tonnes per year by 2100 [8].
Ordinary Portland cement (OPC) is the most commonly used type of cement [9–10]. Within OPC, tricalcium silicate (C3S) is the predominant phase, accounting for 50wt%–70wt% [11]. The rapid hydration of C3S generates a large amount of calcium silicate hydrate (C–S–H) gels, which contribute significantly to the early strength of cement by forming a strong structure [12]. Therefore, the hydration process of C3S is considered crucial for the strength development of cement-based materials and has received extensive attention from scholars [13–15].
Research on the four periods of C3S cement hydration—initial reaction, induction, acceleration, and deceleration—has provided insights into the cement hydration process [16]. However, despite these advancements, the initial reaction period remains the least understood due to its significantly high reaction rate [17] and multiple processes involved, such as water molecule adsorption, proton exchange, dissolution, and precipitation [18], making experimental characterization challenging. Nevertheless, knowledge about the initial reaction period is an essential part of a comprehensive understanding of the cement hydration process.
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Xinhang Xu, Zirou Liu, Dino Spagnoli, Danial Jahed Armaghani, Chongchong Qi (2025). Adsorption mechanism of multiple water molecules on tricalcium silicate (001) surface: A DFT study. Int. Journal of Minerals, Metallurgy and Materials (矿物冶金与材料学报). https://doi.org/10.1007/s12613-024-3073-7
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Frequently Asked Questions
What is the main objective of this DFT study?
The main objective is to investigate the adsorption mechanism of multiple water molecules on the M3-C3S(001) surface at various coverage levels using first-principles calculations, extending the understanding from single to multiple water molecule adsorption.
How does water coverage affect adsorption energies on C3S surfaces?
As water coverage increases, the total adsorption energy becomes more negative, indicating stronger overall binding, but the average adsorption energy per water molecule becomes more positive, suggesting weaker per-molecule interaction due to water–water repulsion.
What role does dissociative adsorption play in the hydration of tricalcium silicate?
Dissociative adsorption, where water molecules split to form Ca–OH bonds, facilitates the detachment of calcium from covalent oxygen, which is significant for the initial hydration process and the eventual formation of C–S–H gels.
Why is the study of multiple water molecule adsorption important for cement science?
Because real cement hydration involves many water molecules, not just single molecules. Understanding coverage effects and water–water interactions is crucial for accurately modeling and optimizing cement hydration and strength development.
What are the practical implications of this research for the construction industry?
The insights into the initial hydration mechanism can help in designing better cement formulations and curing conditions to enhance early strength and durability, contributing to more sustainable and efficient construction materials.
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