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PreprintCited by 24CO2 Sequestration and Geologic InteractionsCalcium Carbonate Crystallization and InhibitionCrystallization and Solubility Studies

Solution additives promoting the onset of MgCO3 nucleation

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Toroz, Dimitrios, Song, Fu, Uddin, Amira, Chass, Gregory A., Di Tommaso, Devis·2021·Crystal Growth & Design
DOI 10.26434/chemrxiv-2021-kl62lPMC PMC9073943

Preprint — published as 10.1021/acs.cgd.1c01525 · Paper page

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Abstract

Formed via aqueous carbonation of Mg2+ ions, the crystallization of magnesite (MgCO3) is a promising carbon capture and reuse technology, albeit limited by the slow precipitation of MgCO3. Although magnesite is naturally abundant, forming at low temperature conditions, its production is an energy-intensive process due to the temperatures required to prevent the formation of hydrated phases. The principle difficulty arises from the very strong Mg2+···H2O interaction, raising barriers to dehydration. Using atomistic simulations, we have investigated the influence of thirty additive anions (Xn–, n = 1–3), ranging from simple halides to more complex molecules, on the first two steps of MgCO3 aggregation from solution: Mg2+ dehydration and Mg2+∙∙∙CO32– pairing. We have computed the thermodynamic stability of solvent shared ion pairs, Mg2+···H2O···Xn–, and contact ion pairs, Mg2+···Xn–, with Mg2+ to reveal the propensity of solution additives to inhibit Mg2+∙∙∙CO32– formation. We have determined the stabilization of undercoordinated hydrated Mg2+ states with a vacant coordination site to which CO32– can bind, subsequently initiating MgCO3 nucleation or Mg2+ incorporation into the crystal lattice. Extensive molecular dynamics simulations of electrolyte solutions containing Na2CO3 with different sources of Mg2+, MgCl2, MgSO4 and Mg(CH3COO)2, further shows that the degree of dehydration of Mg2+ and the structure of prenucleation MgCO3 clusters changes depending on the type counterion. Through a fundamental understanding of the role of solution additives in the mechanism of Mg2+ dehydration, our computational study can rationalize previously reported experimental observation of the effect of solvation environments on the growth of magnesite. This understanding may contribute to identifying solution composition conditions that could promote the low-temperature CO2 conversion into MgCO3.

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  • Few works in the last decade have demonstrated precipitation of amorphous magnesium carbonates employing variable precursors (MgCl2•6H2O, MgO, and anhydrous MgCl2).

    “As a matter of fact, few works produced in the last decade have demonstrated the precipitation of amorphous magnesium carbonates employing variable precursors (MgCl 2 •6H 2 O, 85 MgO, 86,87 and anhydrous MgCl 2 17,88 ).”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [88]

  • The majority of works considers that the amorphous phase precipitates with a sphere of coordinated water (2 to 4 water molecules, resembling the composition of hydrated Mg carbonate phases).

    “The majority of the works considers that the amorphous phase precipitates with a sphere of coordinated water (2 to 4 water molecules, resembling the composition of hydrated Mg carbonate phases), 85,87,88”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [88]

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Authors
Toroz, D., Song, F., Uddin, A., Chass, G. A., & Di Tommaso, D.
Affiliations
  • Queen Mary University of London (GB)
  • University of British Columbia (CA)
  • Queen Mary University of London
Corresponding author
Chass, Gregory A.
ORCID
Venue
Crystal Growth & Design
Publisher
American Chemical Society (ACS)
Published
2021-07-22
Volume
22
Issue
5
Pages
3080-3089
ISSN
1528-7483 (ISSN-L)
DOI
10.26434/chemrxiv-2021-kl62l
PMC
PMC9073943
OpenAlex
W4226411523
Cited by
24
References
37
Citations by year
2026: 9 · 2025: 5 · 2024: 5 · 2023: 4 · 2022: 1
FWCI
1.14
Type
journal article
Language
en
Open access
Licence
Locations
  • Crystal Growth & Design (publishedVersion, cc-by)
  • ChemRxiv (acceptedVersion, cc-by-nc-nd)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • Queen Mary Research Online (Queen Mary University of London) (submittedVersion, cc-by)
Funders
  • Queen Mary University of London
  • McMaster University
  • Department for Business, Energy and Industrial Strategy, UK Government
  • European Commission (294766)
  • National Research Foundation (2016R1A3B1908336)
  • Agence de l'Environnement et de la Maîtrise de l'Energie
  • Ministerio de Economía y Competitividad
  • Ministry of Science, ICT and Future Planning (2016R1A3B1908336)
  • National Research Foundation of Korea (2016R1A3B1908336)
  • University of British Columbia
  • Engineering and Physical Sciences Research Council (L000202, (EP/L000202), EP/T022213/1, EP/P020194, EP/P020194/1 and EP/T022213/1, EP/P020194/1, EP/T022213)
  • Natural Environment Research Council
  • Agencia Estatal de Investigación
Topics
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
  • Physical Sciences › Materials Science › Materials Chemistry › Crystallization and Solubility Studies
Keywords
magnesite, CO2 capture, aqueous carbonation, prenucleation clusters, contact ion pairs, counterion effects, CO2 mineralization, low-temperature CO2 conversion, electrolyte solutions

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