A long-term study on structural changes in calcium aluminate silicate hydrates

Sonya Barzgar*, Yiru Yan, Mohamed Tarik, Jorgen Skibsted, Christian Ludwig, Barbara Lothenbach

*Corresponding author for this work

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Production of blended cements in which Portland cement is combined with supplementary cementitious materials (SCM) is an effective strategy for reducing the CO2 emissions during cement manufacturing and achieving sustainable concrete production. However, the high Al2O3 and SiO2 contents of SCM change the chemical composition of the main hydration product, calcium aluminate silicate hydrate (C–A–S–H). Herein, spectroscopic and structural data for C–A–S–H gels are reported in a large range of equilibration times from 3 months up to 2 years and Al/Si molar ratios from 0.001 to 0.2. The 27Al MAS NMR spectroscopy and thermogravimetric analysis indicate that in addition to the C–A–S–H phase, secondary phases such as strätlingite, katoite, Al(OH)3 and calcium aluminate hydrate are present at Al/Si ≥ 0.03 limiting the uptake of Al in C–A–S–H. More secondary phases are present at higher Al concentrations; their content decreases with equilibration time while more Al is taken up in the C–A–S–H phase. At low Al contents, Al concentrations decrease strongly with time indicating a slow equilibration, in contrast to high Al contents where a clear change in Al concentrations over time was not observed indicating that the equilibrium has been reached faster. The 27Al NMR studies show that tetrahedrally coordinated Al is incorporated in C–A–S–H and its amount increases with the amount of Al present in the solution.

Original languageEnglish
Article number243
JournalMaterials and Structures/Materiaux et Constructions
Number of pages22
Publication statusPublished - Dec 2022


  • Aluminum
  • Blended cement
  • CO emission
  • C–A–S–H
  • Equilibration time
  • NMR


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