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Cited by 49Carbon Dioxide Capture TechnologiesCO2 Sequestration and Geologic InteractionsCarbon dioxide utilization in catalysis

Integrated CO2 Capture and Removal via Carbon Mineralization with Inherent Regeneration of Aqueous Solvents

Liu, Meishen, Hohenshil, Allison, Gadikota, Greeshma·2021·Energy & Fuels
DOI 10.1021/acs.energyfuels.0c04346
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Abstract

Rapid scientific advancements are needed to remove CO 2 from our emissions. In this context, novel molecularly integrated pathways to capture and remove CO 2 as environmentally benign and solid inorganic carbonates are needed. In this study, single-step integrated CO 2 capture and carbonate formation pathways with the inherent regeneration of the aqueous solvents for CO 2 capture are reported. The effectiveness of solvents, such as monoethanolamine (MEA), sodium glycinate (NaGly), 2-amino-2-methylpropanol (AMP), and 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), on the carbon mineralization of CaO, CaSiO 3, and MgO is investigated. Experiments are performed at solvent concentrations of 0, 0.5, 1.0, and 2.5 equiv mol/L at 75 °C, p CO 2 of 1 atm with 15 wt % solid, and a reaction time of 3 h in a continuously stirred environment. The highest extents of carbon mineralization of CaO, CaSiO 3, and MgO are 98.9% at 5 M MEA, 43.40% at 2 M AMP, and 87.50% at 1 M NaGly. High concentrations of aqueous solvents, such as AMP and DBU, exceeding 1 M inhibit carbon mineralization due to the formation of viscous, gel-like fluidic environments that limit transport behavior. Stable calcite and metastable aragonite and vaterite phases result from the carbon mineralization of CaO and CaSiO 3 materials. Metastable hydrated magnesium carbonate phases, such as MgCO 3 ·3H 2 O (nesquhonite), MgCO 3 ·5H 2 O (lansfordite), and hydromagnesite [Mg 5 (CO 3 ) 4 (OH) 2 ·4H 2 O], result from the carbon mineralization of MgO. Overall, significant enhancement in carbon mineralization is achieved using integrated CO 2 capture and carbon mineralization routes with the inherent regeneration of the solvent, as opposed to the base case, where only water is used.

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Crossref · 10.1021/acs.energyfuels.0c04346

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  • Glycine can induce formation of carbamic acid followed by the respective carbamate and zwitterionic glycine.

    “For example, glycine can induce the formation of the carbamic acid followed by the production of the respective carbamate and zwitterionic glycine.115,116”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [115]

  • Methods for CO2 mineralization can be broadly separated into three main approaches: pH-swing, elevated temperatures and CO2 pressures, and reaction of Mg bearing silicates with CO and H2O via water-gas shift reaction to produce magnesium carbonates and H2(g).

    “These contradictions have motivated the development of different methods for CO 2 mineralization which can be broadly separated in three main approaches: the first based on pH-swing, the second based on the usage of elevated temperatures and CO 2 pressures, 105,115 and the third reacts Mg bearing silicates with CO and H 2 O via water-gas shift reaction to produce magnesium carbonates and H 2 (g).”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [115]

  • The rate-limiting reaction will depend on the synthetic conditions of temperature, partial pressure, pH, ionic strength, the type of the reactional fluids and the accessible surface area.

    “The ratelimiting reaction will depend on the synthetic conditions of temperature, partial pressure, pH, ionic strength, the type of the reactional fluids and the accessible surface area.115”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [115]

  • Although methods of carbon mineralization are based on thermodynamically downhill reactions, the role of multiphase reaction pathways and the respective kinetics are not completely understood yet.

    “Although such methods of carbon mineralization are based on thermodynamically downhill reactions (Table 7), the role of multiphase reaction pathways and the respective kinetics are not completely understood yet.115”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [115]

  • The use of amines as catalysts has been demonstrated, indicating a promising pathway to avoid energy and/or chemical intensive processes.

    “In a third approach, the use of amines as catalysts have been demonstrated, indicating a promising pathway to avoid energy and/or chemical intensive processes.115”

    From Mechanisms of Mg carbonates precipitation and implications for CO <sub>2</sub> capture and utilization/storage (2023) · cites this paper as [115]

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Authors
Liu, M., Hohenshil, A., & Gadikota, G.
Affiliations
Cornell University (US)
Corresponding author
Gadikota, Greeshma
ORCID
Venue
Energy & Fuels
Publisher
American Chemical Society (ACS)
Published
2021-04-22
Volume
35
Issue
9
Pages
8051-8068
ISSN
  • 0887-0624 (ISSN-L)
  • 1520-5029
DOI
10.1021/acs.energyfuels.0c04346
OpenAlex
W3157860005
Cited by
49
References
73
Citations by year
2026: 6 · 2025: 10 · 2024: 15 · 2023: 7 · 2022: 9 · 2021: 2
FWCI
3.53
Type
journal article
Language
en
Open access
closed
Licence
Locations
Energy & Fuels (publishedVersion)
Topics
  • Physical Sciences › Engineering › Mechanical Engineering › Carbon Dioxide Capture Technologies
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
Keywords
CO2 capture, carbon mineralization, solvent regeneration, monoethanolamine, sodium glycinate, DBU, calcium oxide, calcium silicate, magnesium oxide, hydrated magnesium carbonate, calcite, aragonite, vaterite, hydromagnesite

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