CO2 adsorption on calcium oxide: An atomic-scale simulation study

SURFACE SCIENCE

卷:606

Article

Besson, R.¹  Vargas, M. Rocha^2,3  Favergeon, L.² 

[1] Univ Sci & Technol Lille, Unite Mat & Transformat, CNRS UMR 8207, F-59655 Villeneuve Dascq, France

[2] Ecole Natl Super Mines, Lab Proc Milieux Granulaires, CNRS FRE 3312, Ctr SPIN, F-42023 St Etienne, France

[3] Inst Super Tecn, Dept Engn Quim, P-1049001 Lisbon, Portugal

关键词: Density functional calculations;    Carbon dioxide adsorption;    Thermodynamic modelling;   

DOI  :  10.1016/j.susc.2011.11.016

来源: Elsevier

【 摘 要 】

We present a detailed study of CO2 adsorption on CaO, by means of atomic-scale simulations relying on Density Functional Theory. Combining ab initio thermodynamics of the CO2 gas phase and a thorough analysis of its interaction with the oxide, we build an orientation-sensitive adsorption model, which demonstrates that low coverage by the gas is expected in a wide range of working conditions, including the domain of stability of CaCO3 calcite. Investigation of the interactions between the adsorbed molecules reinforces this conclusion. Our work thus provides a strong hint that calcite nucleation should occur by a localised mechanism, discarding the possibility of collective surface transformation. (C) 2011 Elsevier B.V. All rights reserved.

【 授权许可】

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