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The influence of slightly and highly soluble carbonate salts on phase relations in hydrated calcium aluminate cements

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Abstract

The addition of slightly (CaCO3) and highly soluble (Na2CO3) carbonate salts is expected to favor the formation of carboaluminate phases in hydrated calcium aluminate cements (CACs). A multi-method approach including X-ray diffraction, thermogravimetric analysis, and thermodynamic calculations is applied to highlight that the “conversion phenomena” in CACs cannot be mitigated by the formation of carboaluminate phases (monocarboaluminate: Mc and hemicarboaluminate: Hc) which are anticipated to form following the addition of carbonate salts. Here, carboaluminate phase formation is shown to depend on three factors: (1) water availability, (2) carbonate content of the salts, and their ability to mobilize CO3 2− species in solution, and (3) lime content associated with the carbonate salt. The latter two factors are linked to the composition and solubility of the carbonate agent. It is concluded that limestone (CaCO3), despite being a source of calcium and carbonate species, contributes only slightly to carboaluminate phase formation due to its low solubility and slow dissolution rate. Soluble carbonate salts (Na2CO3) fail to boost carboaluminate phase formation as the availability of Ca2+ ions and water are limiting. Detailed thermodynamic calculations are used to elucidate conditions that affect the formation of carboaluminate phases.

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Notes

  1. Standard cement chemistry notation is used. As per this simplified notation: C = CaO, A = Al2O3, F = Fe2O3, S = SiO2, CS = CaSO4·2H2O, H = H2O, and \( \overline{\text{C}} = {\text{CO}}_{2} \).

  2. Certain commercial materials and equipment are identified to adequately specify experimental procedures. In no case does, such identification implies recommendation or endorsement by University of California, Los Angeles, École des Mines d’Alès, or Arizona State University, nor does it imply that the items identified are necessarily the best available for the purpose.

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Acknowledgements

The authors acknowledge the financial support for this research provisioned by the University of California, Los Angeles (UCLA), and National Science Foundation (CMMI: 1066583). The authors also acknowledge the provision of materials by OMYA A.G. and Kerneos Aluminate Technologies. The contents of this paper reflect the views and opinions of the authors who are responsible for the accuracy of the datasets presented herein. This research was conducted in the Laboratory for the Chemistry of Construction Materials (LC2) and Molecular Instrumentation Center (MIC) at the University of California, Los Angeles (UCLA). As such, the authors gratefully acknowledge support that has made these laboratories and their operations possible.

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Authors and Affiliations

  1. Laboratory for the Chemistry of Construction Materials, Department of Civil and Environmental Engineering, University of California, Los Angeles, CA, USA

    Guillermo Puerta-Falla, Aditya Kumar, Melanie Rivera, Gabriel Falzone & Gaurav Sant

  2. Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA

    Magdalena Balonis

  3. Institute for Technology Advancement, University of California, Los Angeles, CA, USA

    Magdalena Balonis

  4. Centre des Matériaux de l’École des Mines d’Alès (C2MA), École des mines d’Alès, Alès, France

    Gwenn Le Saout

  5. School of Sustainable Engineering and the Built Environment (SSBE), Arizona State University, Tempe, AZ, USA

    Narayanan Neithalath

  6. California Nanosystems Institute (CNSI), University of California, Los Angeles, CA, USA

    Gaurav Sant

Authors
  1. Guillermo Puerta-Falla
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  2. Magdalena Balonis
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  3. Gwenn Le Saout
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  4. Aditya Kumar
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  6. Gabriel Falzone
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  7. Narayanan Neithalath
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  8. Gaurav Sant
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Correspondence to Gaurav Sant.

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Puerta-Falla, G., Balonis, M., Le Saout, G. et al. The influence of slightly and highly soluble carbonate salts on phase relations in hydrated calcium aluminate cements. J Mater Sci 51, 6062–6074 (2016). https://doi.org/10.1007/s10853-016-9912-9

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  • DOI: https://doi.org/10.1007/s10853-016-9912-9

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