Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

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

doi:10.1021/acs.jpcc.4c04953

Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

Journal Article · Sat Dec 21 00:00:00 EST 2024 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.4c04953· OSTI ID:2483947

^[1]; Moseley, Brittany ^[2]; ^[1]; ^[1]; ^[1]; ^[1]; ^[3]; ^[4]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Roane State Community College, Harriman, TN (United States)
Pennsylvania State Univ., University Park, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

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.

🛈

This content will become publicly available on Sun Dec 21 00:00:00 EST 2025

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2483947

Journal Information:: Journal of Physical Chemistry. C, Vol. XXX; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Isothermal Time-Series Determination of the Rate of Diffusion of Water in Pachuca Obsidian* Anovitz, L. M.; Elam, J. M.; Riciputi, L. R. Archaeometry, Vol. 46, Issue 2 https://doi.org/10.1111/j.1475-4754.2004.00159.x	journal	May 2004
Reviewing direct air capture startups and emerging technologies Wang, Eryu; Navik, Rahul; Miao, Yihe Cell Reports Physical Science, Vol. 5, Issue 2 https://doi.org/10.1016/j.xcrp.2024.101791	journal	February 2024
Raman microspectroscopy of some iron oxides and oxyhydroxides de Faria, D. L. A.; Venâncio Silva, S.; de Oliveira, M. T. Journal of Raman Spectroscopy, Vol. 28, Issue 11 https://doi.org/10.1002/(SICI)1097-4555(199711)28:11<873::AID-JRS177>3.0.CO;2-B	journal	November 1997
Hydration of MgO: Reaction Kinetics and pH Control on Brucite Crystal Morphology Pettauer, Michael; Baldermann, Andre; Eder, Stefan Crystal Growth & Design, Vol. 24, Issue 7 https://doi.org/10.1021/acs.cgd.4c00243	journal	March 2024
Hydration of MgO(100) Surface Promoted at ⟨011⟩ Steps Sasahara, Akira; Murakami, Tatsuya; Tomitori, Masahiko The Journal of Physical Chemistry C, Vol. 119, Issue 15 https://doi.org/10.1021/acs.jpcc.5b01759	journal	April 2015
Investigation of the MgO?Fe system using the M�ssbauer effect Bhide, V. G.; Tambe, B. R. Journal of Materials Science, Vol. 4, Issue 11 https://doi.org/10.1007/BF00555310	journal	November 1969
First principles simulations of MgO(100) surface hydration at ambient conditions Sassi, Michel; Rosso, Kevin M. Physical Chemistry Chemical Physics, Vol. 26, Issue 3 https://doi.org/10.1039/D3CP04848A	journal	January 2024
Characterization of Iron Oxides Commonly Formed as Corrosion Products on Steel Oh, Sei J.; Cook, D. C.; Townsend, H. E. Hyperfine Interactions, Vol. 112, Issue 1/4, p. 59-66 https://doi.org/10.1023/A:1011076308501	journal	January 1998
Thermodynamics of iron oxides: Part III. Enthalpies of formation and stability of ferrihydrite (∼Fe(OH)₃), schwertmannite (∼FeO(OH)_3/4(SO₄)_1/8), and ε-Fe₂O₃ Majzlan, J.; Navrotsky, A.; Schwertmann, U. Geochimica et Cosmochimica Acta, Vol. 68, Issue 5, p. 1049-1059 https://doi.org/10.1016/S0016-7037(03)00371-5	journal	March 2004
Mossbauer study of brucite (Mg, Fe) (OH)2 Binfu, Xu; Yilong, Chen Wuhan University Journal of Natural Sciences, Vol. 4, Issue 1 https://doi.org/10.1007/BF02827620	journal	March 1999
Calcite Growth Rates As a Function of Aqueous Calcium-to-Carbonate Ratio, Saturation Index, and Inhibitor Concentration: Insight into the Mechanism of Reaction and Poisoning by Strontium Bracco, Jacquelyn N.; Grantham, Meg C.; Stack, Andrew G. Crystal Growth & Design, Vol. 12, Issue 7 https://doi.org/10.1021/cg300350k	journal	June 2012
Potentiometric Mass Titrations: Experimental and Theoretical Establishment of a New Technique for Determining the Point of Zero Charge (PZC) of Metal (Hydr)Oxides Bourikas, Kyriakos; Vakros, John; Kordulis, Christos The Journal of Physical Chemistry B, Vol. 107, Issue 35 https://doi.org/10.1021/jp035123v	journal	August 2003
On the morphology of dislocation etch-pits on cube faces of MgO in acids Borecka, B.; Sangwal, K. Journal of Materials Science Letters, Vol. 1, Issue 8 https://doi.org/10.1007/BF00726489	journal	August 1982
Iron Removal using Magnesium Oxide O'Connor, John T.; Benson, Barrett E. Journal of the Sanitary Engineering Division, Vol. 96, Issue 6 https://doi.org/10.1061/JSEDAI.0001202	journal	December 1970
Development and evaluation of a thermodynamic dataset for phases of interest in CO2 mineral sequestration in basaltic rocks Aradóttir, E. S. P.; Sonnenthal, E. L.; Jónsson, H. Chemical Geology, Vol. 304-305 https://doi.org/10.1016/j.chemgeo.2012.01.031	journal	April 2012
Kinetics and product of ferrous iron oxygenation in aqueous systems Sung, Windsor.; Morgan, James J. Environmental Science & Technology, Vol. 14, Issue 5 https://doi.org/10.1021/es60165a006	journal	May 1980
Raman Spectra of Possible Corrosion Products of Iron Thibeau, Richard J.; Brown, Chris W.; Heidersbach, Robert H. Applied Spectroscopy, Vol. 32, Issue 6 https://doi.org/10.1366/000370278774330739	journal	November 1978
Simultaneous ex-situ CO 2 mineral sequestration and hydrogen production from olivine-bearing mine tailings Kularatne, Kanchana; Sissmann, Olivier; Kohler, Eric Applied Geochemistry, Vol. 95 https://doi.org/10.1016/j.apgeochem.2018.05.020	journal	August 2018
Constraining the Origins of the Magnetism of Lepidocrocite (γ-FeOOH): A Mössbauer and Magnetization Study Guyodo, Yohan; Bonville, Pierre; Till, Jessica L. Frontiers in Earth Science, Vol. 4 https://doi.org/10.3389/feart.2016.00028	journal	March 2016
Precipitation in the Mg-carbonate system—effects of temperature and CO2 pressure Hänchen, Markus; Prigiobbe, Valentina; Baciocchi, Renato Chemical Engineering Science, Vol. 63, Issue 4 https://doi.org/10.1016/j.ces.2007.09.052	journal	February 2008
Manganese (Mn) Concentrations and the Mn-Fe Relationship in Shallow Groundwater: Implications for Groundwater Monitoring Hamer, Kay; Gudenschwager, Imke; Pichler, Thomas Soil Systems, Vol. 4, Issue 3 https://doi.org/10.3390/soilsystems4030049	journal	August 2020
57Fe quadrupole interaction and superparamagnetism of Fe2+ in crystals of MgO Simkin, D. J.; Ficalora, P. J.; Bernheim, R. A. Physics Letters, Vol. 19, Issue 7 https://doi.org/10.1016/0031-9163(65)90763-8	journal	December 1965
Investigation on the Mechanisms of Mg(OH)₂ Dehydration and MgO Hydration by Near-Infrared Spectroscopy Kondo, Atsushi; Kurosawa, Ryo; Ryu, Junichi The Journal of Physical Chemistry C, Vol. 125, Issue 20 https://doi.org/10.1021/acs.jpcc.1c01470	journal	May 2021
Preparation of rod‐like MgO by simple precipitation method for CO₂ capture at ambient temperature Tuan, Vu Anh; Lee, Chang Ha Vietnam Journal of Chemistry, Vol. 56, Issue 2 https://doi.org/10.1002/vjch.201800013	journal	April 2018
Thermodynamics of Fe oxides: Part II. Enthalpies of formation and relative stability of goethite (α-FeOOH), lepidocrocite (γ-FeOOH), and maghemite (γ-Fe ₂ O ₃ ) Majzlan, Juraj; Grevel, Klaus-Dieter; Navrotsky, Alexandra American Mineralogist, Vol. 88, Issue 5-6 https://doi.org/10.2138/am-2003-5-614	journal	May 2003
Frustrated Coulombic and Cation Size Effects on Nanoscale Boehmite Aggregation: A Tumbler Small- and Ultra-Small-Angle Neutron Scattering Study Anovitz, L. M.; Huestis, P.; Rampal, N. The Journal of Physical Chemistry C, Vol. 126, Issue 9 https://doi.org/10.1021/acs.jpcc.1c10580	journal	February 2022
Temperature and common-ion effect on magnesium oxide (MgO) hydration Amaral, L. F.; Oliveira, I. R.; Salomão, R. Ceramics International, Vol. 36, Issue 3 https://doi.org/10.1016/j.ceramint.2009.12.009	journal	April 2010
Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging Weber, Juliane; Bracco, Jacquelyn N.; Poplawsky, Jonathan D. Crystal Growth & Design, Vol. 18, Issue 9 https://doi.org/10.1021/acs.cgd.8b00839	journal	July 2018
Fourier-transform infrared and X-ray diffraction analyses of the hydration reaction of pure magnesium oxide and chemically modified magnesium oxide Kurosawa, Ryo; Takeuchi, Masato; Ryu, Junichi RSC Advances, Vol. 11, Issue 39 https://doi.org/10.1039/D1RA04290D	journal	January 2021
Mineral processing water treatment using magnesium oxide Schiller, Joseph E.; Tallman, Daniel N.; Khalafalla, Sanaa E. Environmental Progress, Vol. 3, Issue 2 https://doi.org/10.1002/ep.670030216	journal	May 1984
Templating Growth of a Pseudomorphic Lepidocrocite Microshell at the Calcite–Water Interface Yuan, Ke; Lee, Sang Soo; Wang, Jun Chemistry of Materials, Vol. 30, Issue 3 https://doi.org/10.1021/acs.chemmater.7b03921	journal	January 2018
Ambient weathering of magnesium oxide for CO2 removal from air McQueen, Noah; Kelemen, Peter; Dipple, Greg Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16510-3	journal	July 2020
Effects of γ-Irradiation, Cation Size, and Salt Concentration on the Aggregation of Boehmite Nanoplatelets Huestis, Patricia L.; Anovitz, Lawrence M.; Kolesnikov, Alexander I. The Journal of Physical Chemistry C, Vol. 127, Issue 10 https://doi.org/10.1021/acs.jpcc.2c07749	journal	March 2023
Structural Transformations in the Decomposition of Mg(OH)₂ and MgCO₃ Kim, M. G.; Dahmen, U.; Searcy, Alan W. Journal of the American Ceramic Society, Vol. 70, Issue 3 https://doi.org/10.1111/j.1151-2916.1987.tb04949.x	journal	March 1987
Molecular-scale mechanisms of CO2 mineralization in nanoscale interfacial water films Abdolhosseini Qomi, M. J.; Miller, Q. R. S.; Zare, S. Nature Reviews Chemistry, Vol. 6, Issue 9 https://doi.org/10.1038/s41570-022-00418-1	journal	August 2022
MgO nanocube hydroxylation by nanometric water films Luong, N. Tan; Holmboe, Michael; Boily, Jean-François Nanoscale, Vol. 15, Issue 24 https://doi.org/10.1039/D2NR07140A	journal	January 2023
Growth of High-Purity and Doped Alkaline Earth Oxides: I. MgO and CaO Abraham, M. M.; Butler, C. T.; Chen, Y. The Journal of Chemical Physics, Vol. 55, Issue 8 https://doi.org/10.1063/1.1676658	journal	October 1971
Pilot-scale calcination of limestone in steam-rich gas for direct air capture Erans, María; Nabavi, Seyed Ali; Manović, Vasilije Energy Conversion and Management: X, Vol. 1 https://doi.org/10.1016/j.ecmx.2019.100007	journal	January 2019
Opposing Effects of Impurity Ion Sr ²⁺ on the Heterogeneous Nucleation and Growth of Barite (BaSO ₄ ) Yuan, Ke; Starchenko, Vitalii; Rampal, Nikhil Crystal Growth & Design, Vol. 21, Issue 10 https://doi.org/10.1021/acs.cgd.1c00715	journal	September 2021
Calcination Studies of Magnesium Oxides Eubank, William Roderick Journal of the American Ceramic Society, Vol. 34, Issue 8 https://doi.org/10.1111/j.1151-2916.1951.tb11644.x	journal	August 1951
CO2-water–basalt interaction. Low temperature experiments and implications for CO2 sequestration into basalts Gysi, Alexander P.; Stefánsson, Andri Geochimica et Cosmochimica Acta, Vol. 81 https://doi.org/10.1016/j.gca.2011.12.012	journal	March 2012
Position of Fe ions in MgO crystalline structure Szczerba, Jacek; Prorok, Ryszard; Stoch, Paweł Nukleonika, Vol. 60, Issue 1 https://doi.org/10.1515/nuka-2015-0024	journal	March 2015
Reaction Layer Formation on MgO in the Presence of Humidity Bracco, Jacquelyn N.; Camacho Meneses, Gabriela; Colón, Omar ACS Applied Materials & Interfaces, Vol. 16, Issue 1 https://doi.org/10.1021/acsami.3c14823	journal	December 2023
Comparison of functionalized carbon nanofibers and multi-walled carbon nanotubes as supports for Fe–Co nanoparticles Vidick, Deborah; Herlitschke, Marcus; Poleunis, Claude J. Mater. Chem. A, Vol. 1, Issue 6 https://doi.org/10.1039/C2TA00131D	journal	January 2013
Influence of Iron Substitution and Solution Composition on Brucite Carbonation Vessey, Colton J.; Raudsepp, Maija J.; Patel, Avni S. Environmental Science & Technology, Vol. 58, Issue 18 https://doi.org/10.1021/acs.est.3c08708	journal	April 2024
Application of Raman spectroscopy to identify iron minerals commonly found in mine wastes Das, Soumya; Hendry, M. Jim Chemical Geology, Vol. 290, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2011.09.001	journal	November 2011
Dissolution kinetics of MgO crystals in aqueous acidic salt solutions Sangwal, K. Journal of Materials Science, Vol. 17, Issue 12 https://doi.org/10.1007/BF00752203	journal	December 1982

Similar Records

Templating Growth of a Pseudomorphic Lepidocrocite Microshell at the Calcite–Water Interface

Journal Article · Fri Jan 05 00:00:00 EST 2018 · Chemistry of Materials · OSTI ID:1427507

Yuan, Ke; Lee, Sang Soo; Wang, Jun; +2 more

Related Subjects

granular materials
iron
magnesium oxide
organic reactions
transmission electron microscopy

Influence of Dissolved Iron in Solution on MgO Hydroxylation and Carbonation

Citation Formats

References (47)

Similar Records

Related Subjects