Density Functional Simulation of Adsorption Behavior within the Dicalcium Silicate-Accelerated Carbonation System

Meicheng Zhao, Meijuan Rao, Fazhou Wang, Yong Tao, Linnu Lu

Research output: Journal article publicationJournal articleAcademic researchpeer-review

4 Citations (Scopus)

Abstract

In this study, the adsorption behavior of various molecules, including H2O, CO2, and H2CO3, on the C2S surface in the carbonation system was systematically compared to elucidate the microscopic mechanism in early accelerated carbonation using density functional theory and ab initio molecular dynamics. The electronic structures on β-C2S and γ-C2S surfaces differ, in that the valence band maximum is contributed by the O p orbital and Ca s orbital, respectively. This difference results in different proton-surface interactions. The protons hydroxylated the [SiO4]4-tetrahedra on the β-C2S surface. On the γ-C2S surface, the protons enter the interior surface to form a three-coordination configuration with Ca atoms in addition to bonding with the [SiO4]4-tetrahedra. The adsorption energy for the dissociative adsorption of H2CO3on both β-C2S and γ-C2S surfaces is significantly higher than that of H2O, and the dissociative adsorption configurations are also more stable. CO2only has a strong adsorption tendency on the γ-C2S surface, where it acquires electrons from the surface Ca atoms to become activated. In the molecular adsorption phase, γ-C2S interacts more strongly with CO2, H2CO3, and its dissociation products. copy; 2022 American Chemical Society.

Original languageEnglish
Pages (from-to)16825-16832
Number of pages8
JournalACS Sustainable Chemistry and Engineering
Volume10
Issue number50
DOIs
Publication statusPublished - 19 Dec 2022
Externally publishedYes

Keywords

  • ab initio calculation
  • adsorption
  • carbonation
  • dicalcium silicate
  • thermodynamic

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry
  • General Chemical Engineering
  • Renewable Energy, Sustainability and the Environment

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