The adsorption of mercury-species on relaxed and rumpled CaO (0 0 1) surfaces investigated by density functional theory

Paul Blowers, Bo Gyeong Kim

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

This research examines the importance of several computational choices in modeling mercury species adsorption on calcium oxide surfaces and is the second in a series of papers. The importance of surface relaxation was tested and it was found that adsorption energies changed for HgCl2, moving adsorption from being at the borderline of physisorption and chemisorption to being strongly chemisorbed. Results for Hg and HgCl were unaffected. A second computational choice, that of the cluster or periodic model size was tested in both the plane of the model (4∈×∈4 or 5∈×∈5 model sizes) and for the depth (two or three layers). It was found that the minimum cluster size for handling mercury adsorption was 5∈×∈5 and that only two layers of depth were needed. The energetic results show that rumpled CaO surfaces will only weakly physisorb elemental mercury, but could be used to capture HgCl2 from coal combustion flue gases, which is in agreement with limited experimental data.

Original languageEnglish (US)
Pages (from-to)505-514
Number of pages10
JournalJournal of Molecular Modeling
Volume17
Issue number3
DOIs
StatePublished - Mar 2011

Fingerprint

Mercury
Density functional theory
density functional theory
Adsorption
Mercuric Chloride
adsorption
Surface relaxation
Physisorption
flue gases
Coal combustion
calcium oxides
Chemisorption
Flue gases
Lime
coal
chemisorption
energy

Keywords

  • Adsorption energy
  • DFT
  • Equilibrium constants
  • Mercury
  • Surface relaxation

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Computer Science Applications
  • Computational Theory and Mathematics
  • Catalysis
  • Organic Chemistry
  • Inorganic Chemistry

Cite this

The adsorption of mercury-species on relaxed and rumpled CaO (0 0 1) surfaces investigated by density functional theory. / Blowers, Paul; Kim, Bo Gyeong.

In: Journal of Molecular Modeling, Vol. 17, No. 3, 03.2011, p. 505-514.

Research output: Contribution to journalArticle

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