DFT-D study of single water adsorption on low-index surfaces of calcium silicate phases in cement

Qi, Chongchong; Spagnoli, Dino; Fourie, Andy

doi:10.1016/j.apsusc.2020.146255

Cited by 40 publications

(50 citation statements)

References 49 publications

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“…51,52 The initial structures of molecules and dissociative adsorption are provided in the supporting material (Figure S1), and detailed explanations have been provided in our previous study. 40 Note that the labels H 1 and H 2 were assigned to distinguish between the two H atoms. There was a special type of O atoms in M3-C 3 S that are not directly connected to Si atoms.…”

Section: Methodsmentioning

confidence: 99%

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Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

et al. 2022

J Am Ceram Soc

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The differences in hydration between β-C 2 S and M3-C 3 S, the main phases of silicate cement, have not been fully investigated. In this study, density functional theory calculations were used to investigate the structure and bond order of β-C 2 S and M3-C 3 S before and after the molecular and dissociative adsorption of single water atoms. The unit cell of M3-C 3 S was found to have some O atoms with lower bond orders than those in β-C 2 S, implying higher chemical reactivity of O atoms in M3-C 3 S. The total bond orders of water atoms generally decreased after molecular adsorption, but reductions were minimal, and there were even increases, when the hydrogen bonding among H and surface O atoms was very weak in several M3-C 3 S surfaces. In the case of dissociative adsorption, the bond orders of water O-H hydroxyl tended to increase, and the other bond orders among water atoms decreased sharply, even to zero in some cases. Moreover, the bond order variations of water atoms of β-C 2 S and M3-C 3 S in molecular adsorption were highly correlated with the adsorption energy, with correlation coefficients of 0.9070 and 0.8330, respectively. In both molecular and dissociative adsorption of β-C 2 S and M3-C 3 S, the total bond order among Ca atoms with other surface atoms decreased after the Ca atoms adsorbed water atoms. This phenomenon also appeared in the dissociative adsorption of surface O atoms. In M3-C 3 S, the total strength of the surface O atom bonded to other surface atoms after dissociative adsorption was similar to the strength of the surface O-H hydroxyl bond. The special O atoms in M3-C 3 S showed a clear layered arrangement on the surfaces.

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Section: Methodsmentioning

confidence: 99%

“…Note that PBE has been proven to outperform PBE sol in terms of accuracy on calcium silicate systems. [38][39][40] The comparison of PBE and PBE sol with experimental values is presented in the supporting material (Table S1).…”

Section: Methodsmentioning

confidence: 99%

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

et al. 2022

J Am Ceram Soc

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“…Ca 2 SiO 4 , as the industrial cement clinkers, has been investigated by DFT calculations extensively, and many studies focused on the hydration of Ca 2 SiO 4 phases. Qi et al 22 investigated H 2 O adsorption on low-index surfaces of Ca 2 SiO 4 , indicating that electron are mainly transferred from surface atoms to H 2 O molecule. Wang et al 23 evaluated H 2 O adsorption on β-Ca 2 SiO 4 surfaces and found a dual interaction between H 2 O and β-Ca 2 SiO 4 (100) surface.…”

Section: Introductionmentioning

confidence: 99%

Revealing the different performance of Li₄SiO₄ and Ca₂SiO₄ for CO₂ adsorption by density functional theory

et al. 2022

RSC Adv.

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“…Fortunately, atomistic simulations can tackle these problems. The previous density functional theory (DFT) -based geometry optimization calculations 26 indicated the adsorption of water on the Ca ion impairs the bonds strength between the calcium and oxygen ions on the surface. Claverie et al 27 investigated the proton transfer at the water/Ca3SiO5 interface using ab initio molecular dynamics (AIMD) simulations and found that the hydroxides formed on the surface are highly stable.…”

Section: Introductionmentioning

confidence: 99%

Ab initio mechanism revealing for tricalcium silicate dissolution

Pan

Ming

et al. 2021

Preprint

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Dissolution of mineral in water is ubiquitous in nature and industry, especially for the calcium silicate species. However, the behavior of such a complex chemical reaction is still unclear at atomic level. Here, we show that the ab initio molecular dynamics and metadynamics simulations enable quantitative analyses of reaction pathways, and the thermodynamics and kinetics of calcium ion dissolution from the tricalcium silicate (Ca3SiO5) surface. The calcium sites with different coordination environment leads to different reaction pathways and free energy barriers. The low free energy barriers lead to that the detachment of calcium ions is a ligand exchange and auto-catalytic process. Moreover, the water adsorption, proton exchange and diffusion of water into the surface layer accelerate the leaching of calcium ions from the surface step by step. The discovery in this work thus would be a landmark for revealing the mechanism of cement hydration.

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DFT-D study of single water adsorption on low-index surfaces of calcium silicate phases in cement

Cited by 40 publications

References 49 publications

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Revealing the different performance of Li₄SiO₄ and Ca₂SiO₄ for CO₂ adsorption by density functional theory

Ab initio mechanism revealing for tricalcium silicate dissolution

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DFT-D study of single water adsorption on low-index surfaces of calcium silicate phases in cement

Cited by 40 publications

References 49 publications

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Revealing the different performance of Li4SiO4 and Ca2SiO4 for CO2 adsorption by density functional theory

Ab initio mechanism revealing for tricalcium silicate dissolution

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Revealing the different performance of Li₄SiO₄ and Ca₂SiO₄ for CO₂ adsorption by density functional theory