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

被引：43

作者：

Besson, R. ^{[1
]}

Vargas, M. Rocha ^{[2
,3
]}

Favergeon, L. ^{[2
]}

机构：

[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

来源：

SURFACE SCIENCE | 2012年 / 606卷 / 3-4期

关键词：

Density functional calculations; Carbon dioxide adsorption; Thermodynamic modelling; DECOMPOSITION; CALCINATION; LIMESTONE; MINERALS; CAPTURE; CACO3; MODEL;

D O I：

10.1016/j.susc.2011.11.016

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

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.

引用

页码：490 / 495

页数：6

共 28 条

[11] A shell model for the simulation of rhombohedral carbonate minerals and their point defects [J].