TY - JOUR
T1 - Mineralisation of atmospheric CO2 in hydromagnesite in ultramafic mine tailings – Insights from Mg isotopes
AU - Oskierski, Hans C.
AU - Turvey, Connor C.
AU - Wilson, Siobhan A.
AU - Dlugogorski, Bogdan Z.
AU - Altarawneh, Mohammednoor
AU - Mavromatis, Vasileios
N1 - Funding Information:
H.C.O. thanks the School of Engineering and IT and the College of Science, Health, Engineering and Education, Murdoch University, for financial support via the NSSG and Small Grant schemes, respectively and acknowledges the Murdoch University Facility for Isotopes. H.C.O. also acknowledges the facilities, and the scientific and technical assistance of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy, Characterisation & Analysis, The University of Western Australia, a facility funded by the University, State and Commonwealth Governments. Funding for this work was provided by an Australian Research Council DECRA Fellowship and grants from Carbon Management Canada and the New South Wales Department of Industry to S.A.W., and by the French national programmes INSU-LEFE and INSU-SYSTER to V.M. Work by C.C.T. was supported by an Australian Postgraduate Award. We would like to thank Matthew Fantle, John Hooker, SR Kimmig and the anonymous reviewers for their constructive comments, which have led to significant improvement of the manuscript.
Funding Information:
H.C.O. thanks the School of Engineering and IT and the College of Science, Health, Engineering and Education, Murdoch University, for financial support via the NSSG and Small Grant schemes, respectively and acknowledges the Murdoch University Facility for Isotopes. H.C.O. also acknowledges the facilities, and the scientific and technical assistance of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy, Characterisation & Analysis, The University of Western Australia, a facility funded by the University, State and Commonwealth Governments. Funding for this work was provided by an Australian Research Council DECRA Fellowship and grants from Carbon Management Canada and the New South Wales Department of Industry to S.A.W. and by the French national programmes INSU-LEFE and INSU-SYSTER to V.M. Work by C.C.T. was supported by an Australian Postgraduate Award. We would like to thank Matthew Fantle, John Hooker, SR Kimmig and the anonymous reviewers for their constructive comments, which have led to significant improvement of the manuscript.
Publisher Copyright:
© 2021 Elsevier Ltd
PY - 2021/9/15
Y1 - 2021/9/15
N2 - In this study we present the first Mg isotope data that record the fate of Mg during mineralisation of atmospheric CO2 in ultramafic mine tailings. At the Woodsreef Asbestos Mine, New South Wales, Australia, weathering of ultramafic mine waste sequesters significant amounts of CO2 in hydromagnesite [Mg5(CO3)4(OH)2·4H2O]. Mineralisation of CO2 in above-ground, sub-aerially stored tailings is driven by the infiltration of rainwater dissolving Mg from bedrock minerals present in the tailings. Hydromagnesite, forming on the surface of the tailings, has lower δ26Mg (δ26MgHmgs = −1.48 ± 0.02‰) than the serpentinised harzburgite bedrock (δ26MgSerpentinite = −0.10 ± 0.06‰), the bulk tailings (δ26MgBulk tailings = −0.29 ± 0.03‰) and weathered tailings containing authigenic clay minerals (δ26MgWeathered tailings = +0.28 ± 0.06‰). Dripwater (δ26MgDripwater = −1.79 ± 0.02‰) and co-existing hydromagnesite (δ26MgHmgs = −2.01 ± 0.09‰), forming in a tunnel within the tailings, and nodular bedrock magnesite [MgCO3] (δ26MgMgs = −3.26 ± 0.10‰) have lower δ26Mg than surficial fluid (δ26Mg = −0.36‰) and hydromagnesite. Complete dissolution of source minerals, or formation of Mg-poor products during weathering, is expected to transfer Mg into solution without significant alteration of the Mg isotopic composition. Aqueous geochemical data and modelling of saturation indices, along with Rayleigh distillation and mixing calculations, indicate that the 26Mg-depletion in the drip water, relative to surficial water, is the result of brucite dissolution and/or precipitation of secondary Mg-bearing silicates and cannot be assigned to bedrock magnesite dissolution. Our results show that the main mineral sources of Mg in the tailings (silicate, oxide/hydroxide and carbonate minerals) are isotopically distinct and that the Mg isotopic composition of fluids and thus of the precipitating hydromagnesite reflects both isotopic composition of source minerals and precipitation of Mg-rich secondary phases. The consistent enrichment and depletion of 26Mg in secondary silicates and carbonates, respectively, underpins the use of the presented hydromagnesite and fluid Mg isotopic compositions as a tracer of Mg sources and pathways during CO2 mineralisation in ultramafic rocks.
AB - In this study we present the first Mg isotope data that record the fate of Mg during mineralisation of atmospheric CO2 in ultramafic mine tailings. At the Woodsreef Asbestos Mine, New South Wales, Australia, weathering of ultramafic mine waste sequesters significant amounts of CO2 in hydromagnesite [Mg5(CO3)4(OH)2·4H2O]. Mineralisation of CO2 in above-ground, sub-aerially stored tailings is driven by the infiltration of rainwater dissolving Mg from bedrock minerals present in the tailings. Hydromagnesite, forming on the surface of the tailings, has lower δ26Mg (δ26MgHmgs = −1.48 ± 0.02‰) than the serpentinised harzburgite bedrock (δ26MgSerpentinite = −0.10 ± 0.06‰), the bulk tailings (δ26MgBulk tailings = −0.29 ± 0.03‰) and weathered tailings containing authigenic clay minerals (δ26MgWeathered tailings = +0.28 ± 0.06‰). Dripwater (δ26MgDripwater = −1.79 ± 0.02‰) and co-existing hydromagnesite (δ26MgHmgs = −2.01 ± 0.09‰), forming in a tunnel within the tailings, and nodular bedrock magnesite [MgCO3] (δ26MgMgs = −3.26 ± 0.10‰) have lower δ26Mg than surficial fluid (δ26Mg = −0.36‰) and hydromagnesite. Complete dissolution of source minerals, or formation of Mg-poor products during weathering, is expected to transfer Mg into solution without significant alteration of the Mg isotopic composition. Aqueous geochemical data and modelling of saturation indices, along with Rayleigh distillation and mixing calculations, indicate that the 26Mg-depletion in the drip water, relative to surficial water, is the result of brucite dissolution and/or precipitation of secondary Mg-bearing silicates and cannot be assigned to bedrock magnesite dissolution. Our results show that the main mineral sources of Mg in the tailings (silicate, oxide/hydroxide and carbonate minerals) are isotopically distinct and that the Mg isotopic composition of fluids and thus of the precipitating hydromagnesite reflects both isotopic composition of source minerals and precipitation of Mg-rich secondary phases. The consistent enrichment and depletion of 26Mg in secondary silicates and carbonates, respectively, underpins the use of the presented hydromagnesite and fluid Mg isotopic compositions as a tracer of Mg sources and pathways during CO2 mineralisation in ultramafic rocks.
KW - CO mineralisation
KW - Hydromagnesite
KW - Magnesium isotopes
KW - Mg-isotopes
KW - Mine tailings
KW - Mineral carbonation
KW - Ultramafic rock
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U2 - 10.1016/j.gca.2021.06.020
DO - 10.1016/j.gca.2021.06.020
M3 - Article
AN - SCOPUS:85109755108
SN - 0016-7037
VL - 309
SP - 191
EP - 208
JO - Geochimica et Cosmochimica Acta
JF - Geochimica et Cosmochimica Acta
ER -