3D crystalline phase and pore structure evolution upon CO₂ exposure in sodium sulfate-activated cement pastes

The effects of CO₂ exposure on sodium sulfate-activated blast furnace slag cement paste have been characterised by X-ray (attenuation) computed tomography revealing changes in micron-scale pore structure, and X-ray diffraction computed tomography (XRD-CT) elucidating changes in the spatial distribution of crystalline and semi-crystalline phases. Accelerated carbonation reduced ettringite volumes and induced formation of hydrotalcite, demonstrating the critical role of Mg-Al-SO₄-layered double hydroxide phases in the CO₂ uptake of these cements. These changes yield a refinement of small pores and increase the overall porosity, reaching values comparable to those of blended Portland cements. Formation factor values were determined considering the pore solution electrical resistivity, calculated from thermodynamic modelling, and the porosity. A correlation between simulated tortuosity and porosity is proposed to estimate the diffusion tortuosity and formation factor of sodium sulfate-activated slag pastes. This approach represents a significant step forward for assessing carbonation resistance and CO₂ uptake capacity of cementitious pastes.