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Advancements in enforced C2S wet carbonation: Leveraging δ13C isotope tracking for reaction insights

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Singer, Marie, van Geldern, Robert, Barth, Johannes A.C., Jansen, Daniel·2024·Journal of CO2 Utilization
DOI 10.1016/j.jcou.2024.102924
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Abstract

This study concerns wet carbonation of β-C 2 S (Ca 2 SiO 4 ) in a closed system at 23 °C. The progress of carbonation was detected by quantitative X-ray diffraction (QXRD) and thermogravimetric analysis (TGA). Further measurements of pH and ion concentrations as well as modelling carbon species and saturation indices were done. Additionally, stable carbon isotope ratios ( δ 13 C) in CO 2 , dissolved inorganic carbon (DIC) and carbonate phases were measured. The aim of this study was to investigate δ 13 C isotope values during C 2 S carbonation. If a systematic fractionation of carbon isotopes occurs during the reaction, it can help to quantify the carbonation reaction. During the carbonation process over 48 h, we found carbon isotope distributions from the gaseous phase to the solution and ultimately to the solid phase. Calculations confirm the direct relation of δ 13 C values to the carbonation progress. With this, stable isotope measurements offer a promising tool to monitor the reaction progress in-situ . • Use of stable carbon isotopes to track carbonation of β-C 2 S in a closed system. • Fractionation of δ 13 C during carbonation reaction. • Carbon isotope distributions from gaseous to fluid and ultimately solid phase. • Stable carbon isotope measurements as tool to monitor carbonation reaction in-situ.

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  • There is a slight deviation between the modelled isotope value of the newly formed calcite (-25.3‰) and the final measured value after the experiment (-27‰).

    “This is reflected by the slight deviation between the modelled isotope value of the newly formed calcite ( -25.3 ‰ ) and the final measured value after the experiment ( -27 ‰ [38]).”

    From Isotope chemistry to trace carbon mineralization in construction materials (2026) · cites this paper as [38]

    Section 3.3 (p. 5) reports a measured δ¹³C value for solid CaCO₃ of 27.0‰ after 48 hours, although the sign is absent in our copy. The retrieved passages do not give a modelled value of −25.3‰ for newly formed calcite or state the claimed deviation. (LLM, conf=0.82)

    Experimental — accuracy not yet measured

  • In closed systems, both CO2 gas partial pressure and isotope values of CO2 evolve upon progressive carbonation.

    “In contrast, in closed systems both CO2 gas partial pressure as well as isotope values of CO2 evolve upon progressive carbonation [38].”

    From Isotope chemistry to trace carbon mineralization in construction materials (2026) · cites this paper as [38]

    The paper reports that gaseous CO2 isotope values changed during carbonation in a closed system (section 4.3, p. 6). It also reports a decrease in CO2 gas volume, but the cited passages do not establish that CO2 partial pressure changed (sections 2.3.1, p. 2, and 4.1, p. 6). (LLM, conf=0.85)

    Experimental — accuracy not yet measured

  • Reported literature data show enrichment of 13C in the solid phase during carbonation under high CO2 concentrations.

    “This observation matches with reported literature data that show enrichment of 13 C in the solid phase during carbonation under high CO2 concentrations [35 -38].”

    From Isotope chemistry to trace carbon mineralization in construction materials (2026) · cites this paper as [38]

  • Enhanced aqueous carbonation of C2S (belite) under a 100% CO2 gas phase undergoes a distinct fractionation of carbon isotopes, with heavier 13C isotopes preferentially incorporated into the solid phase and resulting in depletion of 13C in the gas phase.

    “As demonstrated in Figure 1, enhanced aqueous carbonation of C₂S (Ca 2 SiO4, belite) undergoes a distinct fractionation of carbon isotopes. Under experimental conditions involving a 100% CO₂ gas phase, the heavier ¹³C isotopes are preferentially incorporated into the solid phase. This selective incorporation in turn results in a depletion of ¹³C in the gas phase.”

    From Isotope chemistry to trace carbon mineralization in construction materials (2026) · cites this paper as [38]

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Authors
Singer, M., van Geldern, R., Barth, J. A. C., & Jansen, D.
Affiliations
Friedrich-Alexander-Universität Erlangen-Nürnberg (DE)
Corresponding author
Singer, Marie
ORCID
Venue
Journal of CO2 Utilization
Publisher
Elsevier BV
Published
2024-10
Volume
88
Pages
102924
ISSN
2212-9820 (ISSN-L)
DOI
10.1016/j.jcou.2024.102924
OpenAlex
W4402435736
Cited by
2
References
3
Citations by year
2026: 2
FWCI
0.23
Type
journal article
Language
en
Open access
Licence
Locations
  • Journal of CO2 Utilization (publishedVersion, cc-by)
  • OPUS FAU (Kooperativer Bibliotheksverbund Berlin-Brandenburg (KOBV), on behalf of the Universitätsbibliothek Erlangen-Nürnberg) (submittedVersion, cc-by)
Funders
  • German Research Foundation
  • Federal Ministry of Education and Research Bonn Office
Topics
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Engineering › Civil and Structural Engineering › Concrete and Cement Materials Research
  • Physical Sciences › Engineering › Mechanical Engineering › Carbon Dioxide Capture Technologies
Keywords
wet carbonation, calcium silicate hydrate, β-C2S, carbon isotope fractionation, CO2 mineralization, dissolved inorganic carbon, carbonate phases, saturation index

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