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This work focuses on the water-montmorillonite interaction under variable atmospheric conditions in order to characterize the interlamellar space (IS) configuration for possible use in the context of geological barrier for radioactive and industrial waste confinement. Atmospheric stress is achieved by applying, for Na-rich montmorillonite, a water sorption/desorption constraint, created at the laboratory scale. This hydrological disturbance allows the “demolition” of the clay history and to highlight the clay hydrous performance. The structural analysis is achieved using modeling of XRD profiles, which allowed us to determine the optimal structural parameters describing the IS configuration along the c∗ axis. During the “in situ” XRD analysis, a sorption/desorption cycle is envisaged by variation of the relative humidity rate (%RH) from the saturated condition (94 %RH) towards extremely dry ones (2-3 %RH). Qualitatively, a new hydration hysteresis behavior of the “stressed” sample appears. Structural analysis achieved before and after perturbation allowed us to identify, respectively, the homogeneous hydration states, the hydrous transition domains, and the hydration heterogeneity degree. This latter parameter is characterized, quantitatively, by variable relative abundances of mixed-layer structure (MLS) population discerned over a wide explored RH range. Using the optimum structural parameter, the water molecule distribution versus the applied hydrous strain was quantified.

Discretization of the Water Uptake Process of Na-Montmorillonite Undergoing Atmospheric Stress: XRD Modeling Approach