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Grating-based X-ray dark-field tomography is a promising technique for biomedical and materials research. Even if the resolution of conventional X-ray tomography does not suffice to resolve relevant structures, the dark-field signal provides valuable information about the sub-pixel microstructural properties of the sample. Here, we report on the potential of X-ray dark-field imaging to be used for time-resolved three-dimensional studies. By repeating consecutive tomography scans on a fresh cement sample, we were able to study the hardening dynamics of the cement paste in three dimensions over time. The hardening of the cement was accompanied by a strong decrease in the dark-field signal pointing to microstructural changes within the cement paste. Furthermore our results hint at the transport of water from certain limestone grains, which were embedded in the sample, to the cement paste during the process of hardening. This is indicated by an increasing scattering signal which was observed for two of the six tested limestone grains. Electron microscopy images revealed a distinct porous structure only for those two grains which supports the following interpretation of our results. When the water filled pores of the limestone grains empty during the experiment the scattering signal of the grains increases.

Enhanced damage due to the alkali-silica reaction (ASR) in concrete exposed to deicing salt (NaCl) is usually attributed to binding of chloride ions in the hydration products of cement. To balance charge, OH -ions are released into the concrete pore solution which increases alkalinity. However, during NaCl ingress a decrease in the OH -concentration of the concrete pore solution due to potassium leaching would reduce SiO 2 solubility and therefore ASR damage. The present work combines expansion measurements with pore solution analysis by ICP-OES and XRD measurements on concretes and hydrated cement pastes. Solubility equilibria calculations were performed with the hydrogeochemical simulation program PHREEQC. The investigations show that the OH -concentration of the pore solution is mainly lowered by potassium leaching during NaCl ingress. The OH -concentration also decreases owing to the formation of Friedel's salt from ettringite which is associated with the release of sulphate. Although the OH -concentration with NaCl is lower, ASR damage is intensified and the silicon concentration in the pore solution is higher. Higher silicon solubility is explained by the higher total alkali concentration which increases surface silicate solubility, the formation of an aqueous complex NaHSiO 3 0 and a higher ionic strength. These effects promote the sensitivity of silicate minerals to ASR, the formation of alkali silica gel and finally ASR damage.