Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

Juliane Weber; Brittany Moseley; Ke Yuan; Barbara R. Evans; Vitalii Starchenko; Elena Tajuelo Rodriguez; Dong Youn Chung; Matthew G. Boebinger; Michael A. McGuire; George Yumnam; Raphael P. Hermann; Lawrence M. Anovitz; Andrew G. Stack

doi:10.1021/acs.jpcc.4c04953

Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

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Abstract

MgO (periclase) is a promising material for direct air capture of CO₂ using a mineral looping process, but it is unknown how impurities in the environment will affect the CO₂ uptake and hence process economics. Here, we investigated the effects of dissolved iron on the extents of MgO hydroxylation and subsequent carbonation reactions to determine if this has a beneficial or detrimental effect. On single-crystal MgO, dissolved iron prevented hydration of MgO to Mg(OH)₂ (brucite) and instead formed a shell of lepidocrocite (γ-FeOOH). This did not passivate the MgO as dissolution below the shell was observed. During hydroxylation of MgO powders in the presence of dissolved iron, formation of brucite containing Fe(II) was observed. In addition, formation of nanoscale iron oxides containing Fe(III) was observed using magnetometry and Mössbauer spectroscopy. Subsequent carbonation experiments showed increased carbonation of MgO hydroxylated in the presence of iron. Our results indicate that the presence of dissolved solute impurities during hydroxylation may be beneficial for carbonation of hydroxylated MgO.

Original language	English
Pages (from-to)	194-204
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	129
Issue number	1
DOIs	https://doi.org/10.1021/acs.jpcc.4c04953
State	Published - Jan 9 2025

Funding

This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. We would like to thank James Kolopus for providing the MgO single-crystal samples used in this study. Portions of this work (Raman characterization) were generated using instrumentation supported by the National Nuclear Security Administration. TEM characterization was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Work performed by BM (part of single-crystal experiments and in situ light microscopy experiments) was supported in part by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS) under the Science Undergraduate Laboratory Internships program. This manuscript has been coauthored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Funding was provided by DOE BES-MSE.

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Weber, J., Moseley, B., Yuan, K., Evans, B. R., Starchenko, V., Tajuelo Rodriguez, E., Chung, D. Y., Boebinger, M. G., McGuire, M. A., Yumnam, G., Hermann, R. P., Anovitz, L. M., & Stack, A. G. (2025). Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation. Journal of Physical Chemistry C, 129(1), 194-204. https://doi.org/10.1021/acs.jpcc.4c04953

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title = "Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation",

abstract = "MgO (periclase) is a promising material for direct air capture of CO2 using a mineral looping process, but it is unknown how impurities in the environment will affect the CO2 uptake and hence process economics. Here, we investigated the effects of dissolved iron on the extents of MgO hydroxylation and subsequent carbonation reactions to determine if this has a beneficial or detrimental effect. On single-crystal MgO, dissolved iron prevented hydration of MgO to Mg(OH)2 (brucite) and instead formed a shell of lepidocrocite (γ-FeOOH). This did not passivate the MgO as dissolution below the shell was observed. During hydroxylation of MgO powders in the presence of dissolved iron, formation of brucite containing Fe(II) was observed. In addition, formation of nanoscale iron oxides containing Fe(III) was observed using magnetometry and M{\"o}ssbauer spectroscopy. Subsequent carbonation experiments showed increased carbonation of MgO hydroxylated in the presence of iron. Our results indicate that the presence of dissolved solute impurities during hydroxylation may be beneficial for carbonation of hydroxylated MgO.",

author = "Juliane Weber and Brittany Moseley and Ke Yuan and Evans, \{Barbara R.\} and Vitalii Starchenko and \{Tajuelo Rodriguez\}, Elena and Chung, \{Dong Youn\} and Boebinger, \{Matthew G.\} and McGuire, \{Michael A.\} and George Yumnam and Hermann, \{Raphael P.\} and Anovitz, \{Lawrence M.\} and Stack, \{Andrew G.\}",

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doi = "10.1021/acs.jpcc.4c04953",

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AU - Weber, Juliane

AU - Moseley, Brittany

AU - Yuan, Ke

AU - Evans, Barbara R.

AU - Starchenko, Vitalii

AU - Tajuelo Rodriguez, Elena

AU - Chung, Dong Youn

AU - Boebinger, Matthew G.

AU - McGuire, Michael A.

AU - Yumnam, George

AU - Hermann, Raphael P.

AU - Anovitz, Lawrence M.

AU - Stack, Andrew G.

PY - 2025/1/9

Y1 - 2025/1/9

N2 - MgO (periclase) is a promising material for direct air capture of CO2 using a mineral looping process, but it is unknown how impurities in the environment will affect the CO2 uptake and hence process economics. Here, we investigated the effects of dissolved iron on the extents of MgO hydroxylation and subsequent carbonation reactions to determine if this has a beneficial or detrimental effect. On single-crystal MgO, dissolved iron prevented hydration of MgO to Mg(OH)2 (brucite) and instead formed a shell of lepidocrocite (γ-FeOOH). This did not passivate the MgO as dissolution below the shell was observed. During hydroxylation of MgO powders in the presence of dissolved iron, formation of brucite containing Fe(II) was observed. In addition, formation of nanoscale iron oxides containing Fe(III) was observed using magnetometry and Mössbauer spectroscopy. Subsequent carbonation experiments showed increased carbonation of MgO hydroxylated in the presence of iron. Our results indicate that the presence of dissolved solute impurities during hydroxylation may be beneficial for carbonation of hydroxylated MgO.

AB - MgO (periclase) is a promising material for direct air capture of CO2 using a mineral looping process, but it is unknown how impurities in the environment will affect the CO2 uptake and hence process economics. Here, we investigated the effects of dissolved iron on the extents of MgO hydroxylation and subsequent carbonation reactions to determine if this has a beneficial or detrimental effect. On single-crystal MgO, dissolved iron prevented hydration of MgO to Mg(OH)2 (brucite) and instead formed a shell of lepidocrocite (γ-FeOOH). This did not passivate the MgO as dissolution below the shell was observed. During hydroxylation of MgO powders in the presence of dissolved iron, formation of brucite containing Fe(II) was observed. In addition, formation of nanoscale iron oxides containing Fe(III) was observed using magnetometry and Mössbauer spectroscopy. Subsequent carbonation experiments showed increased carbonation of MgO hydroxylated in the presence of iron. Our results indicate that the presence of dissolved solute impurities during hydroxylation may be beneficial for carbonation of hydroxylated MgO.

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SP - 194

EP - 204

JO - Journal of Physical Chemistry C

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Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

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