Effect of Lithium Doping on MgO Hydroxylation and Carbonation

Camacho Meneses, Gabriela; Yuan, Ke; Stack, Andrew G.; Evans, Barbara R.; Moseley, Brittany; Ievlev, Anton V.; Borisevich, Albina Y.; Hernandez Penagos, Pedro J.; Bañuelos, Jose L.; Chung, Dong Youn; Adapa, Sai; Einkauf, Jeffrey D.; Stubbs, Joanne E.; Eng, Peter J.; Boebinger, Matthew G.; Bracco, Jacquelyn N.; Weber, Juliane

doi:10.1021/acsearthspacechem.5c00345

Title: Effect of Lithium Doping on MgO Hydroxylation and Carbonation

Journal Article · Tue Mar 03 00:00:00 UTC 2026 · ACS Earth and Space Chemistry

DOI: https://doi.org/10.1021/acsearthspacechem.5c00345 · OSTI ID:3022118

Camacho Meneses, Gabriela ^[1];

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City Univ. of New York (CUNY), NY (United States). Queens College
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Roane State Community College, Harriman, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Texas at El Paso, TX (United States)
Pennsylvania State Univ., University Park, PA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
Univ. of Chicago, IL (United States)
City Univ. of New York (CUNY), NY (United States)

Recovery of magnesium from brines can potentially be used to source MgO (periclase) as a CO₂ sorbent or for Mg-based cements. However, it is not clear how common impurities in brines, such as lithium, affect the resulting MgO reactivity. Here, to test the effect of lithium incorporation on MgO reactivity for hydration and carbonation, we combined computational simulations with experiments. Experimentally altered (Mg,Li)O with a low dopant concentration (0.012 ± 0.002% w/w Li) was characterized using synchrotron-based X-ray scattering and high-resolution electron microscopy to measure reaction layer formation on (Mg,Li)O. Single-crystal X-ray diffraction analysis of (Mg,Li)O demonstrates that the incorporation of lithium leads to the formation of oxygen vacancies. The presence of vacancies is likely causing faster hydroxylation rates as predicted by ab initio molecular dynamics simulations. However, the faster hydroxylation rates likely lead to faster passivation of the surface because we observe thinner reaction layers on (Mg,Li)O samples both over short time periods (30 days) and over long time periods (28 years). After 28 years, the reaction layer on the (Mg,Li)O sample was less than one-third of the thickness of that of the pure MgO sample. In addition, over 30 days, reaction layers on (Mg,Li)O samples primarily formed at steps rather than on terraces, in contrast to our previous observations on MgO. Based on our results, naturally occurring impurities in MgO modify its reactivity even at very low concentrations and need to be considered for accurate reaction rate prediction for application of MgO as a CO₂ sorbent or in cements.

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

Sponsoring Organization:: National Energy Research Scientific Computing Center (NERSC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; SC0019108

OSTI ID:: 3022118

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 3 Vol. 10; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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X-ray reflectivity
electron microscopy
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molecular dynamics simulations
periclase

Title: Effect of Lithium Doping on MgO Hydroxylation and Carbonation

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