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An atomistic Monte Carlo investigation on the Solid-Liquid phasetransition in BCC iron: The role of boundary conditions
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Materials Process Science.
(English)In: Computational materials science, ISSN 0927-0256Article in journal (Other academic) Submitted
URN: urn:nbn:se:kth:diva-26339OAI: diva2:371869
QS 20120328Available from: 2010-11-23 Created: 2010-11-23 Last updated: 2012-03-28Bibliographically approved
In thesis
1. Theoretical and experimental studies of surface and interfacial phenomena involving steel surfaces
Open this publication in new window or tab >>Theoretical and experimental studies of surface and interfacial phenomena involving steel surfaces
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The present work was initiated to investigate the surface- and interfacial phenomena for iron and slag/iron systems. The aim was to understand the mechanism of the effect of surface active elements on surface and interfacial properties. In the present work, the adsorption of oxygen and sulfur on iron surface as well as adatom surface movements were studied based on the ab initio method. BCC iron melting phenomena and sulfur diffusion in molten iron were investigated by Monte Carlo simulations. The impact of oxygen potential on interfacial mass transfer was carried out by X-ray sessile drop method.

Firstly, the structural, electronic and magnetic properties as well as thermodynamic stability were studied by Density functional theory (DFT). The hollow site was found to be the most stable adsorption site both for oxygen and sulfur adsorbed on iron (100) surface, which is in agreement with the experiment. The relaxation geometries and difference charge density of the different adsorption systems were calculated to analyze the interaction and bonding properties between Fe and O/S. It can be found that the charge redistribution was related to the geometry relaxation. In addition, the sulfur coverage is considered from a quarter of one monolayer (1ML) to a full monolayer. It was found that the work function and its change Δφ increased with S coverage, in very good agreement with experiment. Due to a recent discussion regarding the influence of charge transfer on Δφ, it is shown in the present work that the increase in Δφ can be explained by the increasing surface dipole moment as a function of S coverage. S strongly interacts with the surface Fe layer and decreases the surface magnetic moment as the S coverage increases.

Secondly, a two dimensional (2D) gas model based on density functional calculations combined with thermodynamics and statistical physics, was proposed to simulate the movement of the surface active elements, viz. oxygen and sulfur atoms on the Fe(100) surface. The average velocity of oxygen and sulfur atoms was found to be related to the vibration frequencies and energy barrier in the final expression developed. The calculated results were based on the density function and thermodynamics & statistical physics theories. In addition, this 2D gas model can be used to simulate and give an atomic view of the complex interfacial phenomena in the steelmaking refining process.

A distance dependent atomistic Monte Carlo model was developed for studying the iron melting phenomenon as well as effect of sulfur on molten iron surface. The effect of boundary conditions on the melting process of an ensemble of bcc iron atoms has been investigated using a Lennard-Jones distance dependent pair potential. The stability of melting process was energetically and spatially analyzed under fixed wall and free surface conditions and the effects of short and long-range interactions were discussed. The role of boundary conditions was significantly reduced when long-range interactions were used in the simulation. This model was further developed for investigating the effect of sulfur on molten iron surface. A combination of fixed wall and free surface boundary condition was found to well-represent the molten bath configuration while considering the second nearest neighbor interactions. Calculations concerning the diffusion of sulfur on molten surface were carried out as a function of temperature and sulfur concentration. Our results show that sulfur atoms tended to diffuse away from the surface into the liquid bulk and the diffusion rate increased by increasing temperature.

Finally, impact of oxygen potential on sulfur mass transfer at slag/metal interface, was carried out by X-ray sessile drop method. The movement of sulfur at the slag/metal interface was monitored in dynamic mode at temperature 1873 K under non-equilibrium conditions. The experiments were carried out with pure iron and CaO-SiO2-Al2O3-FeO slag (alumina saturated at the experimental temperature) contained in alumina crucibles with well-controlled partial pressures of oxygen and sulfur. As the partial pressure of oxygen increased, it was found that interfacial velocity as well as the oscillation amplitude increased. The thermo-physical and thermo-chemical properties of slag were also found to influence interfacial velocity.


Place, publisher, year, edition, pages
Stockholm: KTH, 2010. 56 p.
Sulfur, Oxygen, Adsorption, Iron surface, ab initio calculations, Adsorption energy, Work function, Difference charge density, Magnetic properties, Thermodynamic stability, Average velocity, Monte Carlo simulation, X-ray sessile drop method, Mass transfer, Interfacial velocity
National Category
Metallurgy and Metallic Materials
urn:nbn:se:kth:diva-26194 (URN)978-91-7415-796-3 (ISBN)
Public defence
2010-12-08, Sal F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (English)
QC 20101123Available from: 2010-11-23 Created: 2010-11-19 Last updated: 2010-11-23Bibliographically approved

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