The purpose of this article is to investigate the carbonation mechanism of CH and C-S-H within type-I cement-based materials in terms of kinetics, microstructure changes and water released from hydrates during carbonation. Carbonation tests were performed under accelerated conditions (10% CO 2 , 25• C and 65± 5% RH). Carbonation profiles were assessed by destructive and non-destructive methods such as phenolphthalein spray test, thermogravimetric analysis, and mercury intrusion porosimetry (destructive), as well as gamma-ray attenuation (non-destructive). Carbonation penetration was carried out at different ages from 1 to 16 weeks of CO 2 exposure on cement pastes of 0.45 and 0.6 w/c, as well as on mortar specimens (w/c = 0.50 and s/c = 2). Combining experimental results allowed us to improve the understanding of C-S-H and CH carbonation mechanism. The variation of molar volume of C-S-H during carbonation was identified and a quantification of the amount of water released during CH and C-S-H carbonation was performed.

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