Magnesium-based cement is one of the most interesting eco-sustainable alternatives to standard cementitious binders. The reasons for the interest towards this material are twofold: (i) its production process, using magnesium silicates, brine or seawater, dramatically reduces CO₂ emissions with respect to Portland cement production, and (ii) it is very well suited to applications in radioactive waste encapsulation. In spite of its potential, assessment of the structural properties of its binder phase (magnesium silicate hydrate or M–S–H) is far from complete, especially because of its amorphous character. In this work, a comprehensive structural characterization of M–S–H was obtained using a multi-technique approach, including a detailed solid-state NMR investigation and, in particular, for the first time, quantitative ²⁹Si solid-state NMR data. M–S–H was prepared through room-temperature hydration of highly reactive MgO and silica fume and was monitored for 28 days. The results clearly evidenced the presence in M–S–H of “chrysotile-like” and “talc-like” sub-nanometric domains, which are approximately in a 1 : 1 molar ratio after long-time hydration. Both these kinds of domains have a high degree of condensation, corresponding to the presence of a small amount of silanols in the tetrahedral sheets. The decisive improvement obtained in the knowledge of M–S–H structure paves the way for tailoring the macroscopic properties of eco-sustainable cements by means of a bottom-up approach.

The characterization of the structural and dynamic properties of rubber networks is of fundamental importance in rubber science and technology to design materials with optimized mechanical properties. In this work, natural and isoprene rubber networks obtained by curing at three different temperatures (140, 150, and 170 °C) and three different sulfur contents (1, 2, and 3 phr) in the presence of a 3 phr accelerator were studied using a combination of low-field time-domain NMR (TD-NMR) techniques, including ¹H multiple-quantum experiments for the measurement of residual dipolar couplings (D_res), the application of the Carr–Purcell–Meiboom–Gill pulse sequence for the measurement of the transverse magnetization decay and the extraction of ¹H T₂ relaxation times, and the use of field cycling NMR relaxometry for the determination of T₁ relaxation times. The microscopic properties determined by TD-NMR experiments were discussed in comparison with the macroscopic properties obtained using equilibrium swelling, moving die rheometer, and calorimetric techniques. The obtained correlations between NMR observables, crosslink density values, maximum torque values, and glass transition temperatures provided insights into the effects of the vulcanization temperature and accelerator/sulfur ratio on the structure of the polymer networks, as well as on the effects of crosslinking on the segmental dynamics of elastomers. D_res and T₂ were found to show linear correlations with the crosslink density determined by equilibrium swelling, while T₁ depends on the local dynamics of polymer segments related to the glass transition, which is also affected by chemical modifications of the polymer chains occurring during vulcanization.

The peculiar mechanism of cooperative CO₂ adsorption in a perfluorinated Ce^IV-based metal–organic framework with MIL-140 topology is disclosed using a combination of experimental and computational methods.