Kinetics of antigorite dehydroxylation for CO2 sequestration

S. Zahid; H.C. Oskierski; I. Oluwoye; H.E.A. Brand; F. Xia; G. Senanayake; M. Altarawneh; B.Z. Dlugogorski

doi:10.1016/j.mineng.2022.107630

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Kinetics of antigorite dehydroxylation for CO2 sequestration

Journal article

Peer reviewed

Kinetics of antigorite dehydroxylation for CO2 sequestration

S. Zahid, H.C. Oskierski, I. Oluwoye, H.E.A. Brand, F. Xia, G. Senanayake, M. Altarawneh and B.Z. Dlugogorski

Minerals Engineering, Vol.184, Art. 107630

2022

DOI: https://doi.org/10.1016/j.mineng.2022.107630

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Abstract

Heat-treatment of serpentine minerals generates structural amorphicity and increases reactivity during subsequent mineral carbonation, a strategy for large-scale sequestration of CO2. This study employs thermal analyses (TGA-DSC) in conjunction with in-situ synchrotron powder X-ray diffraction (PXRD) to record concurrent mass loss, heat flow, and mineralogical changes during thermal treatment of antigorite. Isoconversional kinetic modelling demonstrates that thermal decomposition of antigorite is a complex multi-step reaction, with activation energies (Eα) varying between 290 and 515 kJ mol−1. We identify three intermediate phases forming during antigorite dehydroxylation, a semi-crystalline chlorite-like phase (γ-metaserpentine) showing an additional reaction pathway for the decomposition of Al2O3-rich antigorite into pyrope, and two distinct amorphous components (α and β-metaserpentine) which convert into forsterite and enstatite at higher temperature, respectively. The combination of isoconversional kinetics with in-situ synchrotron PXRD illustrates, for the first time, that local crystal structure changes, related to intermediate phase and forsterite formation, are responsible for the steep increase in activation energy above 650 °C and only 49% dehydroxylation can be achieved prior to this increase. This suggests that the high thermal stability of Al2O3-rich antigorite would severely limit Mg extraction during application of mineral carbonation under flue gas conditions.

Details

Title: Kinetics of antigorite dehydroxylation for CO2 sequestration
Authors/Creators: S. Zahid (Author/Creator) - Murdoch University
H.C. Oskierski (Author/Creator)
I. Oluwoye (Author/Creator)
H.E.A. Brand (Author/Creator)
F. Xia (Author/Creator)
G. Senanayake (Author/Creator)
M. Altarawneh (Author/Creator)
B.Z. Dlugogorski (Author/Creator)
Publication Details: Minerals Engineering, Vol.184, Art. 107630
Publisher: Elsevier BV
Identifiers: 991005542566407891
Copyright: © 2022 Elsevier Ltd.
Murdoch Affiliation: Harry Butler Institute; School of Mathematics, Statistics, Chemistry and Physics
Language: English
Resource Type: Journal article

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Collaboration types: Domestic collaboration
Citation topics: 2 Chemistry; 2.165 Nanofibers, Scaffolds & Fabrication; 2.165.1082 Calcium Carbonate Crystallization
Web Of Science research areas: Engineering, Chemical; Mineralogy; Mining & Mineral Processing
ESI research areas: Geosciences