Density functional theory study of the decomposition of Mg(OH)2: A lamellar dehydroxylation model

Andrew Chizmeshya; M. J. McKelvy; R. Sharma; Ray Carpenter; H. Bearat

doi:10.1016/S0254-0584(02)00020-2

Density functional theory study of the decomposition of Mg(OH)₂: A lamellar dehydroxylation model

Andrew Chizmeshya, M. J. McKelvy, R. Sharma, Ray Carpenter, H. Bearat

Chemical Engineering

Research output: Contribution to journal › Article › peer-review

26 Scopus citations

Abstract

We present a density functional theory investigation of the decomposition of Mg(OH)₂. Based on recent experiments indicating a lamellar dehydroxylation process we have calculated the energetics, elastic behavior and structural trends of a series of oxyhydroxide intermediates of composition Mg_x+yO_x(OH)_2y representing a solid solution series between brucite (Mg(OH)₂) and periclase (MgO). Using a variationally induced breathing (VIB) ionic approach we find that this broad range of lamellar oxyhydroxide intermediate materials becomes thermodynamically accessible at temperatures near 500°C. The computed dehydroxylation dependence of the compressibility is found to vary dramatically with the initial formation of periclase-like oxide layers displaying an abrupt jump to a value near that of periclase (∼160GPa). In contrast to this very non-linear behavior the basal plane lattice parameter a is found to exhibit a nearly linear (Vegard-like) dependence on hydroxyl content.

Original language	English (US)
Pages (from-to)	416-425
Number of pages	10
Journal	Materials Chemistry and Physics
Volume	77
Issue number	2
DOIs	https://doi.org/10.1016/S0254-0584(02)00020-2
State	Published - Jan 15 2003

Keywords

Computer simulation
Density functional theory
Intermediate phases
Mg(OH)
MgO
Oxyhydroxide
Reactivity

ASJC Scopus subject areas

Materials Science(all)
Condensed Matter Physics

Access to Document

10.1016/S0254-0584(02)00020-2

Cite this

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title = "Density functional theory study of the decomposition of Mg(OH)2: A lamellar dehydroxylation model",

abstract = "We present a density functional theory investigation of the decomposition of Mg(OH)2. Based on recent experiments indicating a lamellar dehydroxylation process we have calculated the energetics, elastic behavior and structural trends of a series of oxyhydroxide intermediates of composition Mgx+yOx(OH)2y representing a solid solution series between brucite (Mg(OH)2) and periclase (MgO). Using a variationally induced breathing (VIB) ionic approach we find that this broad range of lamellar oxyhydroxide intermediate materials becomes thermodynamically accessible at temperatures near 500°C. The computed dehydroxylation dependence of the compressibility is found to vary dramatically with the initial formation of periclase-like oxide layers displaying an abrupt jump to a value near that of periclase (∼160GPa). In contrast to this very non-linear behavior the basal plane lattice parameter a is found to exhibit a nearly linear (Vegard-like) dependence on hydroxyl content.",

keywords = "Computer simulation, Density functional theory, Intermediate phases, Mg(OH), MgO, Oxyhydroxide, Reactivity",

author = "Andrew Chizmeshya and McKelvy, {M. J.} and R. Sharma and Ray Carpenter and H. Bearat",

note = "Funding Information: We gratefully acknowledge the National Energy Technology Laboratory of the US Department of Energy for support through grants DE-FG26-98FT40112 and DE-FG26-99FT40580. We also thank the Center for Solid State Science for use of the Goldwater Materials Science Laboratories, including the Materials Facility, and in particular, the Goldwater Materials Visualization Facility.",

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T1 - Density functional theory study of the decomposition of Mg(OH)2

T2 - A lamellar dehydroxylation model

AU - Chizmeshya, Andrew

AU - McKelvy, M. J.

AU - Sharma, R.

AU - Carpenter, Ray

AU - Bearat, H.

N1 - Funding Information: We gratefully acknowledge the National Energy Technology Laboratory of the US Department of Energy for support through grants DE-FG26-98FT40112 and DE-FG26-99FT40580. We also thank the Center for Solid State Science for use of the Goldwater Materials Science Laboratories, including the Materials Facility, and in particular, the Goldwater Materials Visualization Facility.

PY - 2003/1/15

Y1 - 2003/1/15

N2 - We present a density functional theory investigation of the decomposition of Mg(OH)2. Based on recent experiments indicating a lamellar dehydroxylation process we have calculated the energetics, elastic behavior and structural trends of a series of oxyhydroxide intermediates of composition Mgx+yOx(OH)2y representing a solid solution series between brucite (Mg(OH)2) and periclase (MgO). Using a variationally induced breathing (VIB) ionic approach we find that this broad range of lamellar oxyhydroxide intermediate materials becomes thermodynamically accessible at temperatures near 500°C. The computed dehydroxylation dependence of the compressibility is found to vary dramatically with the initial formation of periclase-like oxide layers displaying an abrupt jump to a value near that of periclase (∼160GPa). In contrast to this very non-linear behavior the basal plane lattice parameter a is found to exhibit a nearly linear (Vegard-like) dependence on hydroxyl content.

AB - We present a density functional theory investigation of the decomposition of Mg(OH)2. Based on recent experiments indicating a lamellar dehydroxylation process we have calculated the energetics, elastic behavior and structural trends of a series of oxyhydroxide intermediates of composition Mgx+yOx(OH)2y representing a solid solution series between brucite (Mg(OH)2) and periclase (MgO). Using a variationally induced breathing (VIB) ionic approach we find that this broad range of lamellar oxyhydroxide intermediate materials becomes thermodynamically accessible at temperatures near 500°C. The computed dehydroxylation dependence of the compressibility is found to vary dramatically with the initial formation of periclase-like oxide layers displaying an abrupt jump to a value near that of periclase (∼160GPa). In contrast to this very non-linear behavior the basal plane lattice parameter a is found to exhibit a nearly linear (Vegard-like) dependence on hydroxyl content.

KW - Computer simulation

KW - Density functional theory

KW - Intermediate phases

KW - Mg(OH)

KW - MgO

KW - Oxyhydroxide

KW - Reactivity

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