AbstractThis work is focused on the effects of drying/re-saturation cycles on the structure and components of White Portland Cement (WPC) samples. In particular, WPC of 0.5 water-to-cement ratio was studied by ¹H Nuclear Magnetic Resonance (NMR) Relaxometry. A number of NMR sequences and different data processing methods were applied. Short (14 days of re-saturation) and long (6 months for the whole cycle) sorption cycles were investigated, using two drying methods: oven drying and drying under controlled relative humidity. The evolution during drying/re-saturation processes of interlayer space, gel pores, and bigger pores was followed by both the transverse relaxation times and the intensities of the nuclear magnetization. As a result of drying, reversible and irreversible changes in the pore structure, especially concerning the smaller porosity (interlayer and gel pores), were seen. Likewise, ¹H signals in the crystalline phases of the cement were investigated by the standard Quadrature Echo method and by a more informative analysis based and a proper acquisition and processing of the longitudinal relaxation data. This analysis allowed the signal separation of ¹H nuclei with higher and lower mobility (“solid” components). The NMR signal from this last component was analyzed on the basis of the Pake-Doublet theory in the time domain and two components were clearly detected, and assigned to ¹H nuclei of crystalline water in Ettringite and OH groups in Portlandite. Reversible changes of the solid components of the cement samples were observed. This is a new method to deeply investigate the changes of solid components during sorption cycles.